Amines catalysis using metallic phosphate condensation catalysts having a cyclic structure

ABSTRACT

This invention relates to a process for making amines by condensing an amino compound in the presence of a metallic phosphate condensation catalyst having a cyclic structure or an acyclic structure which is transformed into a cyclic structure during said process. This invention also relates to an alkyleneamines producers composition rich in triethylenetetramine (TETA), tetraethylenepentamine (TEPA) and pentaethylenehexamine (PEHA).

RELATED APPLICATIONS

U.S. patent application Ser. No. 136,615, filed Dec. 22, 1987, commonly-assigned.

The following are related, commonly assigned applications, filed on an even date herewith: U.S. patent application Ser. No. (390,829), U.S. patent application Ser. No. (390,709); U.S. patent application Ser. No. (390,714); U.S. patent application Ser. No. (390,828); and U.S. patent application Ser. No. (390,708); all incorporated herein by reference.

BRIEF SUMMARY OF THE INVENTION

1. Technical Field

This invention relates to a process for making amines by condensing an amino compound in the presence of a metallic phosphate condensation catalyst having a cyclic structure or an acyclic structure which is transformed into a cyclic structure during said process.

This invention also relates to an alkyleneamines producers composition rich in higher polyalkylene polyamines such as triethylenetetramine (TETA), tetraethylenepentamine (TEPA) and pentaethylenehexamine (PEHA).

2. Background of the Invention

There is a substantial body of literature directed to the use of various acid catalysts to effect intramolecular and intermolecular condensation of amino compounds. U.S. Pat. No. 2,073,671 and U.S. Pat. No. 2,467,205 constitute early prior work on the use of acid condensation catalysts to condense amino compounds. U.S. Pat. No. 2,073,671 discusses, in a general fashion, the catalytic intermolecular condensation of alcohols and amines or ammonia using the same phosphate catalysts later favored by U.S. Pat. No. 2,467,205 for the intramolecular condensation of amines. The two patents are not in harmony over the use of other materials as catalysts. To illustrate this point, U.S. Pat. No. 2,073,671 states:

"Alumina, thoria, blue oxide of tungsten, titania, chromic oxide, blue oxide of molybdenum and zirconia have been mentioned in the literature for use as catalysts in carrying out these reactions but their effectiveness is so low that no practical application has been made of their use."

whereas U.S. Pat. No. 2,467,205 in describing the self condensation of ethylenediamine (EDA) under vapor phase conditions, to initially produce ethyleneamines, but after recycle, eventually enerates piperazine through multistep condensation reactions, followed by deamination, recommends "dehydration catalysts" which are thereafter characterized as

"silica gel, titania gel, alumina, thoria, boron phosphate, aluminum phosphate, and the like."

U.S. Pat. No 2,073,671 describes the condensation catalyst in the following terms:

". . . a heated catalyst or contact mass containing phosphorus and especially one or more of the oxygen acids of phosphorus, their anhydrides, their polymers, and their salts; for example, orthophosphoric acid, metaphosphoric acid, pyrophosphoric acid, phosphorous pentoxide, dimetaphosphoric acid, trimetaphosphoric acid, primary ammonium phosphate, secondary ammonium phosphate, normal ammonium phosphate, ammonium metaphosphate, secondary ammonium pyrophosphate, normal ammonium pyrophosphate, aluminum phosphate, aluminum acid phosphate and mixtures of two or more of such materials."

whereas U.S. Pat. No. 2,467,205 describes one of the preferred catalysts as "basic aluminum phosphate".

U.S. Pat. No. 2,454,404 describes the "catalytic deamination of alkylene polyamines" by reacting diethylenetriamine (DETA) vapor over solid catalysts such as activated alumina, bauxite, certain aluminum silicates such as kaolin and oxides of thorium, titanium and zirconium.

U.S. Pat. Nos. 2,073,671 and 2,467,205 demonstrate a common experience in using aluminum phosphate as a condensation catalyst to produce aliphatic amines, and U.S. Pat. Nos. 2,454,404 and 2,467,205 contemplate the other solid catalysts for deamination of amines to make heterocyclic noncyclic amines. In general, the reaction conditions under which deamination to effect cyclization occurs are more severe than those employed for condensation to generate noncyclic molecules, all other factors being comparable.

U.S. Pat. Nos. 4,540,822, 4,584,406 and 4,588,842 depict the use of Group IVB metal oxides as supports for phosphorus catalysts used to effect the condensation of amino compounds with alkanolamines.

U.S. Pat. No. 4,683,335 describes the use of tungstophosphoric acid, molybdophosphoric acid or mixtures deposited on titania as catalysts for the condensation of amines and alkanolamines to make polyalkylenepolyamines.

U.S. Pat. Nos. 4,314,083, 4,316,840, 4,362,886 and 4,394,524 disclose the use of certain metal sulfates as useful catalysts for the condensation of alkanolamine and an amino compound. No distinction is made between the sulfur compounds in respect to catalytic efficacy. Sulfuric acid is as good as any metal sulfate, and all metal sulfates are treated as equivalents. At column 8 of U.S. Pat. No. 4,314,083, it is noted that boron sulfate "gave extremely high selectivity at a low level" of EDA. However, selectivity in general was shown to increase with an increase of EDA relative to MEA in the feed. The only specific metal sulfates disclosed in the patents are antimony sulfate, beryllium sulfate, iron sulfate and aluminum sulfate.

In the typical case of the manufacture of alkyleneamines, mixtures with other alkyleneamines (including a variety of polyalkylenepolyamines and cyclic alkylenepolyamines) are formed. The same holds true when the object of the process is to produce polyalkylenepolyamines whether acyclic or cyclic, in that a variety of amino compounds are also formed. Each of these cyclic and acyclic alkyleneamines can be isolated from the mixture.

The acid catalyzed condensation reaction involving the reaction of an alkanolamine with an amino compound in the presence of an acidic catalyst is believed to proceed through the mechanism of esterifying free surface hydroxyl groups on the acid catalyst with the alkanolamine and/or by protonating the alkanolamine in the presence of the acid catalyst, followed by loss of water and amine condensation of the ester or the hydrated species, as the case may be, to form the alkyleneamine. Illustrative prior art directed primarily to the cyclic polyalkylenepolyamines (heterocyclic polyamines), but not necessarily limited to the aforementioned acid condensation reaction, are: U.S. Pat. Nos. 2,937,176, 2,977,363, 2,977,364, 2,985,658, 3,056,788, 3,231,573, 3,167,555, 3,242,183, 3,297,701, 3,172,891, 3,369,019, 3,342,820, 3,956,329, 4,017,494, 4,092,316, 4,182,864, 4,405,784 and 4,514,567; European Patent Applications 0 069 322, 0 111 928 and 0 158 319; East German Patent No. 206,896; Japanese Patent Publication No. 51-141895; and French Patent No. 1,381,243. The evolution of the art to the use of the acid catalyzed condensation reaction to generate acyclic alkyleneamines, particularly acyclic polyalkylenepolyamines, as the predominant products stemmed from the initial disclosure in U.S. Pat. No. 4,036,881, though earlier patent literature fairly well characterized such an effect without labeling it so, see U.S. Pat. No. 2,467,205, supra. The acid catalysts are phosphorus compounds and the reaction is carried out in the liquid phase. The trend in this catalyst direction was early set as demonstrated by U.S. Pat. Nos. 2,073,671 and 2,467,205, supra. A modification of this route includes the addition of ammonia to the reaction, see, for example, U.S. Pat. No. 4,394,524 and U.S. Pat. No. 4,463,193 for the purpose of converting alkanolamine such as MEA in situ to alkylene amine such as EDA by reaction with ammonia, and the EDA is in situ reacted with MEA according to the process of U.S. Pat. No. 4,036,881 to form alkyleneamines.

A summary of the prior art employing acid catalysts for making alkyleneamines is set forth in Table 1 below.

                                      TABLE 1                                      __________________________________________________________________________     CITATION    CATALYST TYPE    REACTANTS                                         __________________________________________________________________________     U.S. Pat. No. 2,467,205                                                                    Silica gel, titania gel, alumina,                                                               Vapor phase condensation of                                   thoria, aluminum phosphate.                                                                     EDA over a fixed bed of the                                   Preferred catalyst is basic                                                                     catalyst, multipass process                                   aluminum phosphate.                                                                             shifts from polyethylene-                                                      polyamines with the first                                                      few cycles.                                       U.S. Pat. No. 4,036,881                                                                    Phosphorus containing substances                                                                Alkanolamine and alkylene-                                    selected from the group consisting                                                              amine in liquid phase                                         of acidic metal phosphates,                                                                     reaction.                                                     phosphoric acid compounds and                                                  their anhydrides, phosphorus acid                                              compounds and their anhydrides,                                                alkyl or aryl phosphate esters,                                                alkyl or aryl phosphite esters,                                                alkyl or aryl substituted                                                      phosphorus and phosphoric acids                                                wherein said alkyl groups have                                                 from 1 to about 8 carbon atoms and                                             said aryl groups have from 6 to                                                about 20 carbon atoms, alkali                                                  metal monosalts of phosphoric                                                  acid, the thioanalogs of the fore-                                             going, and mixtures of the above.                                  U.S. Pat. No. 4,044,053                                                                    Phosphorus containing substances                                                                Alkanepolyols and alkylene-                                   selected from the group consisting                                                              amine in liquid phase                                         of acidic metal phosphates,                                                                     reaction.                                                     phosphoric acid compounds and                                                  their anhydrides, phosphorus                                                   acid compounds and their                                                       anhydrides, alkyl or aryl                                                      phosphate esters, alkyl or aryl                                                phosphite esters, alkyl or aryl                                                substituted phosphorous acids and                                              phosphoric acids wherein said                                                  alkyl groups have from 1 to about                                              8 carbon atoms and said aryl                                                   groups have from 6 to about 20                                                 carbon atoms, alkali metal mono-                                               salts of phosphoric acid and                                                   mixtures of the above.                                             U.S. Pat. No. 4,314,083                                                                    Salt of a nitrogen or sulfur con-                                                               Alkanolamine and an                                           taining substance or the corres-                                                                alkyleneamine in liquid                                       ponding acid.    phase reaction.                                   U.S. Pat. No. 4,316,840                                                                    Metal nitrates and sulfates                                                                     Reforming linear polyamines.                                  including zirconium sulfate.                                       U.S. Pat. No. 4,316,841                                                                    Phosphate, preferably boron                                                                     Reforming linear polyamines.                                  phosphate.                                                         U.S. Pat. No. 4,324,917                                                                    Phosphorus-containing cation                                                                    Alkanolamine and an alkylene-                                 exchange resin.  amine in liquid phase                                                          reaction.                                         U.S. Pat. No. 4,362,886                                                                    Arsenic, antimony or bismuth                                                                    Alkanolamie and an alkylene-                                  containing compounds. Antimony                                                                  amine in liquid phase                                         sulfate specifically disclosed.                                                                 reaction.                                         U.S. Pat. No. 4,399,308                                                                    Lewis acid halide.                                                                              Alkanolamine and an alkylene-                                                  amine in liquid phase                                                          reaction.                                         U.S. Pat. No. 4,394,524                                                                    Phosphorus-containing substance                                                                 Ammonia, alkanolamine and an                                  or salt of a sulfur-containing                                                                  alkyleneamine in liquid phase                                 substance, or the corresponding                                                                 reaction.                                                     acid.                                                              U.S. Pat. No. 4,448,997                                                                    Reacts alumina with phosphoric                                                                  EDA with MEA                                                  acid, adds ammonium hydroxide.                                     U.S. Pat. No. 4,463,193                                                                    Group IIIB metal acid phosphate.                                                                Ammonia, alkanolamine and                                                      an alkyleneamine.                                 U.S. Pat. No. 4,503,253                                                                    Supported phosphoric acid.                                                                      Ammonia, alkanolamine and                                                      an alkyleneamine.                                 U.S. Pat. No. 4,521,600                                                                    Select hydrogen phosphates and                                                                  Alkanolamine and an alkylene-                                 pyrophosphates.  amine.                                            U.S. Pat. No. 4,524,143                                                                    Phosphorus impregnated onto                                                                     Alkanolamine and an alkylene-                                 zirconium silicate support.                                                                     amine.                                            U.S. Pat. No. 4,540,822                                                                    Phosphorus compound deposited                                                                   Alkanolamine and an alkylene-                                 on a Group IVB metal oxide                                                                      amine, regenerates the                                        support.         catalyst with O.sub.2 -containing                                              gas.                                              U.S. Pat. No. 4,547,591                                                                    Silica-alumina alone or in                                                                      An ethyleneamine and an                                       combination with an acidic                                                                      alkanolamine; ethyleneamines;                                 phosphorus cocatalyst.                                                                          or ammonia and an alkanol-                                                     amine.                                            U.S. Pat. No. 4,550,209                                                                    An intercalatively catalytically                                                                EDA and MEA.                                                  active tetravalent zirconium                                                   polymeric reaction product of an                                               organo phosphonic acid or an                                                   ester thereof with a compound of                                               tetravalent zirconium reactive                                                 therewith.                                                         U.S. Pat. No. 4,552,961                                                                    Phosphorus amide compound.                                                                      Alkyleneamine and alkanolamine                                                 and/or alkylene glycol.                           U.S. Pat. No. 4,555,582                                                                    Phosphorus chemically bonded to                                                                 MEA and EDA.                                                  a zirconium silicate support.                                      U.S. Pat. No. 4,560,798                                                                    Rare earth metal or strontium                                                                   MEA.                                                          acid phosphate.                                                    U.S. Pat. No. 4,578,517                                                                    Group IIIB metal acid phosphate.                                                                Ammonia or p-/s-amine                                                          alkanolamine.                                     U.S. Pat. No. 4,578,518                                                                    Thermally activated, calcined,                                                                  MEA and EDA.                                                  pelleted titania containing                                                    titanium triphosphate. " . . . the                                             titania that was used was . . .                                                anatase." (Col. 9, lines 18-19).                                   U.S. Pat. No. 4,578,519                                                                    Thermally activated, calcined,                                                                  MEA and EDA with optional                                     pelleted titania with chemically                                                                recycle of DETA.                                              bonded phosphorus derived from                                                 polyphosphoric acid.                                               U.S. Pat. No. 4,584,405                                                                    Activated carbon, optionally                                                                    MEA and EDA.                                                  treated to incorporate phosphorus.                                             Activated carbon may be washed                                                 with strong mineral acid to                                                    remove impurities followed by                                                  water wash. Optional treatment                                                 follows.                                                           U.S. Pat. No. 4,584,406                                                                    Pelleted Group IVB metal oxide                                                                  MEA and EDA.                                                  with chemically bonded phosphorus                                              derived from phosphoryl chloride                                               or bromide.                                                        U.S. Pat. No. 4,588,842                                                                    Thermally activated pelleted                                                                    MEA and EDA.                                                  Group IVB metal oxide with                                                     chemically bonded phosphorus.                                      U.S. Pat. No. 4,605,770                                                                    Group IIA or IIIB metal acid                                                                    Alkanolamine and an                                           phosphate.       alkyleneamine "in liquid                                                       phase".                                           U.S. Pat. No. 4,609,761                                                                    Thermally activated pelleted                                                                    MEA and EDA.                                                  titania with chemically bonded                                                 phosphorus.                                                        U.S. Pat. No. 4,612,397                                                                    Thermally activated pelleted                                                                    MEA and EDA.                                                  titania with chemically bonded                                                 phosphorus.                                                        U.S. Pat. No. 4,617,418                                                                    Acid catalysts, mentions "beryl-                                                                Ammonia, alkanolamine and                                     lium sulfate".   an alkyleneamine "under                                                        vapor phase conditions".                          Japanese Patent                                                                            Variety of phosphorus and metal                                                                 Ammonia, alkanolamine and                         Application phosphates including Group IVB                                                                  ethyleneamine, with ammonia/                      #1983-185,871,                                                                             phosphates.      alkanolamine molar ratio                          Publication                  greater than 11.                                  #1985-78,945                                                                   U.S. Pat. No. 4,683,335                                                                    Tungstophosphoric acid, molybdo-                                                                Claims reaction of MEA and                                    phosphoric acid or mixtures                                                                     EDA, but discloses self-                                      deposited on titania. Examples                                                                  condensation reaction of                                      2-7 characterize titania surface                                                                EDA and DETA.                                                 areas of 51, 60 and 120 m.sup.2 /gm.                               Japanese Patent                                                                            Group IVB metal oxide with                                                                      Ammonia and MEA.                                  Application bonded phosphorus.                                                 #1985-078,391,                                                                 Publication                                                                    #1986-236,752                                                                  Japanese Patent                                                                            Group IVB metal oxide with                                                                      Ammonia and MEA.                                  Application bonded phosphorus.                                                 #1985-078,392,                                                                 Publication                                                                    #1986-236,753                                                                  U.S. Pat. No. 4,698,427                                                                    Titania having phosphorus                                                                       Diethanolamine and/or                                         thermally chemically bonded                                                                     hydroxyethyldiethylene-                                       to the surface thereof in the                                                                   triamine in EDA.                                              form of phosphate bonds.                                           U.S. Pat. No. 4,806,517                                                                    Pelleted Group IVB metal oxide                                                                  MEA and EDA.                                                  with phosphorus thermally                                                      chemically bonded to the                                                       surface thereof.                                                   __________________________________________________________________________

The market demand for higher polyalkylene polyamines such as TETA, TEPA and PEHA has been progressively increasing in recent years. These higher polyalkyene polyamines are desirable co-products with DETA. It would be desirable to satisfy the existing demand from a cost standpoint by modifying slightly the commercial processes directed to the manufacture of DETA from the reaction of MEA and EDA or other suitable starting raw materials such as DETA and AEEA, to the production of TETA, TEPA and PEHA as major products.

It would be desirable to have continuously produced compositions, generated by the reaction of MEA and EDA or other suitable starting raw materials such as DETA and AEEA over a fixed bed of a condensation catalyst under commercial conditions, that are rich in TETA, TEPA and PEHA, and that are not disproporationately high in PIP and other cyclics.

It would be very beneficial to have a process which increases one's ability to generate the manufacture of desirable higher polyalkylene polyamine products such as TETA, TEPA and PEHA without generating large amounts of cyclic alkylenepolyamine products. In addition, it would also be desirable to have a process with raw material flexibility which provides the potential to control congener distribution, linear to cyclic selectivity and linear to branched selectivity of the higher polyalkylene polyamines products. As used herein, congener distribution refers to polyalkylene polyamines containing the same number of nitrogen atoms but not necessarily having the same molecular weight or structure.

The above features are provided by this invention.

SUMMARY OF THE INVENTION

This invention relates in general to a process of making amines which comprises condensing an amino compound in the presence of a metallic phosphate condensation catalyst having a cyclic structure or an acyclic structure which is transformed into a cyclic structure during said process. The metallic phosphate condensation catalysts used herein contain sufficient residual bound hydroxyl groups or other groupings which renders catalyst formation possible by loss of water or its chemical equivalent such as ammonium hydroxide.

More particularly, this invention relates to a process of making amines by the (i) intramolecular condensation of an amino compound to an amine having a lower molecular weight or (ii) the intermolecular condensation of an amino compound with one or more of another amino compound or a compound containing an alcoholic hydroxyl group using certain metallic phosphates having a cyclic structure or an acyclic structure which is transformed into a cyclic structure during said process as the condensation catalyst. A preferred process involves the manufacture of alkyleneamines, most desirably higher polyalkylene polyamines, by such condensation reactions utilizing sodium dihydrogen phosphate, disodium dihydrogen pyrophosphate or sodium trimetaphosphate as the condensation catalyst.

The invention further relates to a continuously generated alkyleneamines producers composition comprising, based on 100 percent of the weight of the composition and exclusive of any water and/or ammonia present,

a) greater than about 3.0 weight percent of the combination of TETA and TEPA,

b) greater than about 0.1 weight percent of TEPA,

c) greater than about 3.0 weight percent of TETA,

d) less than about 90.0 weight percent of DETA and/or EDA,

e) less than about 90.0 weight percent of MEA and/or AEEA,

f) less than about 12.5 weight percent of the combination of PIP and AEP,

g) less than about 15.0 weight percent of other polyalkylene polyamines,

h) a TETA+TAEA to PIP+AEP+PEEDA+DAEP+DPE weight ratio of greater than about 0.5,

i) a TEPA+AETAEA to PIP+AEP+PEEDA+DAEP+DPE+AEPEEDA+iAEPEEDA AEDAEP+AEDPE+BPEA weight ratio of greater than about 0.5,

j) a TETA to TAEA weight ratio of greater than about 2.0, and

k) a TEPA to AETAEA weight ratio of greater than about 2.0.

As used herein, the term "amino compound" embraces ammonia and any compound containing nitrogen to which is bonded an active hydrogen. Also, as used herein, the term "oxide" embraces oxides, hydroxides and/or mixtures thereof.

For purposes of this invention, the chemical elements are identified in accordance with the Periodic Table of the Elements, CAS version, Handbook of Chemistry and Physics, 67th Ed., 1986-87, inside cover. Also, for purposes of this invention, Group IIIB metal oxides embraces the lanthanides and actinides.

DETAILED DESCRIPTION

The higher polyalkylene polyamines such as TETA, TEPA and PEHA are very useful commercial products for a variety of applications including fuel oil additives, corrosion inhibitors, fabric softeners, fungicides and others. As indicated above, there is lacking a commercial process for the manufacture of enhanced quantities of TETA, TEPA and PEHA especially as significant products of reaction. There is thus a need for the ability to commercially generate larger production quantities of TETA, TEPA and PEHA and that is the direction of this invention. The process of this invention provides for the reaction of MEA and DETA or other suitable starting raw materials such as EDA and AEEA to produce in a continuous manner a reaction product mixture, termed herein an "alkyleneamines producers composition", in which TETA, TEPA and PEHA are principal products of the reaction.

The process of this invention is distinctive insofar as it achieves the generation of high concentrations of TETA, TEPA and PEHA in a manner which can be suitably employed in a commercial process, particularly a continuous process, for the manufacture of alkyleneamines. In particular, the process of this invention allows the production of TETA, TEPA and PEHA in relatively high yields without generating large amounts of cyclic polyalkylene polyamine products. The process of this invention provides starting raw material flexibility thereby allowing the potential to control congener distribution, linear to cyclic selectivity and linear to branched selectivity of the higher polyalkylene polyamine products.

As indicated above, this invention relates to a process of making amines which comprises condensing an amino compound in the presence of a metallic phosphate condensation catalyst having a cyclic structure or an acyclic structure which is transformed into a cyclic structure during said process.

As also indicated above, this invention relates to a continuously generated alkyleneamines producers composition comprising, based on 100 percent of the weight of the composition and exclusive of any water and/or ammonia present,

a) greater than about 3.0 weight percent of the combination of TETA and TEPA,

b) greater than about 0.1 weight percent of TEPA,

c) greater than about 3.0 weight percent of TETA,

d) less than about 90.0 weight percent of DETA and/or EDA,

e) less than about 90.0 weight percent of MEA and/or AEEA,

f) less than about 12.5 weight percent of the combination of PIP and AEP,

g) less than about 15.0 weight percent of other polyalkylene polyamines,

h) a TETA+TAEA to PIP+AEP+PEEDA+DAEP+DPE weight ratio of greater than about 0.5,

i) a TEPA+AETAEA to PIP+AEP+PEEDA+DAEP+DPE+AEPEEDA+iAEPEEDA+AEDAEP+AEDPE+BPEA weight ratio of greater than about 0.5,

j) a TETA to TAEA weight ratio of greater than about 2.0, and

k) a TEPA to AETAEA weight ratio of greater than about 2.0.

The alkyleneamines producers composition of this invention can be subjected to conventional separations techniques for recovering the individual components of the composition. Such techniques are well known in the art and include, for example, distillation.

This invention contemplates the catalyzed condensation by (i) intramolecular condensation of an amino compound to an amine having a lower molecular weight, and (ii) intermolecular condensation of an amino compound with one or more of another amino compound or a compound containing an alcohol hydroxyl group to an amine having a lower, same or higher molecular weight than the reactants, in the presence of a metallic phosphate condensation catalyst having a cyclic structure or an acyclic structure which is transformed into a cyclic structure during the process. The metallic phosphate condensation catalysts embraced within the scope of this invention can be cyclic or a mixture of cyclic and acyclic and comprise structural units of the formula: ##STR1## wherein M is the same or different and is a substantially insoluble cation, X is the same or different and is oxygen, nitrogen or sulfur, and y is a value of from 1 to about 20 or greater. The preferred metallic phosphate condensation catalysts have a cyclic structure and ionic character and/or ion exchange capacity.

While not wishing to be bound to any particular theory, it is believed that those metallic phosphates encompassed within the scope of this invention having a cyclic structure and possessing ionic character and/or ion exchange capacity exhibit desired catalytic activity and provide desired product selectivity. While the reaction mixture may initially include one or more metallic phosphates other than metallic phosphates having a cyclic structure and possessing ionic character and/or ion exchange capacity, it is believed to be desirable that such metallic phosphates having a cyclic structure and possessing ionic character and/or ion exchange capacity be formed in situ in order to provide desired catalytic activity and product selectivity. In such instances, catalyst preparation conditions or the reaction conditions should allow for the formation of metallic phosphates having a cyclic structure and possessing ionic character and/or ion exchange capacity. Mixtures of metallic phosphates having a cyclic structure and possessing ionic character and/or ion exchange capacity with metallic phosphates having other than a cyclic structure and other than ionic character and/or ion exchange capacity are believed to exhibit desired catalytic activity and provide desired product selectivity.

In accordance with this invention, the metallic phosphate condensation catalyst has a cyclic structure or an acyclic structure which is capable of being transformed into a cyclic structure during the process. The metallic phosphate condensation catalyst can include, for example, metallic orthophosphates (PO₄ ⁻³), metallic pyrophosphates (P₂ O₇ ⁻⁴), metallic polyphosphates (including tripolyphosphates (P₃ O₁₀ ⁻⁵), tetrapolyphosphates (P₄ O₁₃ ⁻⁶), pentapolyphosphates (P₅ O₁₆ ⁻⁷), and higher polyphosphates), metallic metaphosphates (including trimetaphosphates (P₃ O₉ ⁻³), tetrametaphosphates (P₄ O₁₂ ⁻⁴) and other lower and higher metaphosphates) and metallic ultraphosphates (condensed phosphates containing more P₂ O₅ than corresponds to the metaphosphate structure). Corresponding metallic metaphosphimates, metallic phosphoramidates and metallic amido- and imidophosphates of the above may also be used as condensation catalysts in accordance with this invention. Suitable metals which can be incorporated into the metallic phosphate condensation catalyst include, for example, Group IA metals, Group IIA metals, Group IIIB metals, Group IVB metals, Group VB metals, Group VIB metals, Group VIIB metals, Group VIII metals, Group IB metals, Group IIB metals, Group IIIA metals, Group IVA metals, Group VA metals, Group VIA metals and mixtures thereof.

Illustrative of metallic orthophosphate catalysts which may be utilized in this invention include, for example, NaH₂ PO₄, KH₂ PO₄, RbH₂ PO₄, LiH₂ PO₄, MgHPO₄, CaHPO₄, YPO₄, CePO₄, LaPO₄, ThPO₄, MnPO₄, FePO₄, BPO₄, AlPO₄, BiPO₄, Mg(H₂ PO₄)₂, Ba(H₂ PO₄)₂, Mg(NH₄)₂ PO₄, Ca(H₂ PO₄)₂, La(H₂ PO₄)₃ and the like. Illustrative of metallic pyrophosphate catalysts which may be utilized in this invention include, for example, Na₂ H₂ P₂ O₇, K₂ H₂ P₂ O₇, Ca₂ P₂ O₇, Mg₂ P₂ O₇, KMnP₂ O₇, AgMnP₂ O₇, BaMnP₂ O₇, NaMnP₂ O₇, KCrP₂ O₇, NaCrP₂ O₇, Na₄ P₂ O₇, K₄ P₂ O₇, Na₃ HP₂ O₇, NaH₃ P₂ O₇, SiP₂ O₇, ZrP₂ O₇, Na₆ Fe₂ (P₂ O₇)₃, Na₈ Fe₄ (P₂ O₇)₅, Na₆ Cu(P₂ O₇)₂, Na₃₂ Cu₁₄ (NH₄)₂ P₂ O₇, Ca₃₂ Cu₁₄ Na₄ Cu₁₈ (P₂ O₇)₅, Na₂ (NH₄)₂ P₂ O₇, Ca(NH₄)₂ P₂ O₇, Mgh₂ P₂ O₇, Mg(NH₄)₂ P₂ O₇ and the like. Illustrative of metallic polyphosphate catalysts which may be utilized in this invention include, for example, NaSr₂ P₃ O₁₀, NaCa₂ P₃ O₁₀, NaNi₂ P₃ O₁₀, Na₅ P₃ O₁₀, K₅ P₃ O₁₀, Na₃ MgP₃ O₁₀, Na₃ CuP₃ O₁₀, Cu₅ (P₃ O₁₀)₂, Na₃ ZnP₃ O₁₀ , Na₃ CdP₃ O₁₀, Na₆ Pb(P₃ O₁₀)₂, Na₃ CoP₃ O₁₀, K₃ CoP₃ O₁₀, Na₃ NiP₃ O₁₀, K₂ (NH₄)₃ P₃ O₁₀, Ca(NH₄)₂ P₃ O₁₀, La(NH₄)₂ P₃ O₁₀, NaMgH₂ P₃ O₁₀ and the like. Illustrative of metallic metaphosphate catalysts which may be utilized in this invention include, for example, Na₃ P₃ O₉, K₃ P₃ O₉, Ag₃ P₃ O₉, Na₄ P₄ O₁₂, K₄ P₄ O₁₂, Na₂ HP₃ O₉, Na₄ Mg(P₃ O₉)₂, NaSrP₃ O₉, NaCaP₃ O₉, NaBaP₃ O₉, KBaP₃ O₉, Ca₃ (P₃ O₉)₂, Ba(P₃ O₉)₂, Na₂ Ni₂ (P₃ O₉)₂, Na₄ Ni(P₃ O₉)₂, Na₄ Co(P₃ O₉)₂, Na₄ Cd(P₃ O₉)₂ and the like. Illustrative of metallic ultraphosphate catalysts which may be utilized in this invention include, for example, CaP₄ O₁₁, Ca₂ P₆ O₁₇, Na₈ P₁₀ O₂₉, Na₆ P₈ O₂₃, Na₂ CaP₆ O₁₇, Na₂ P₄ O₁₁, NaBaP₇ O₁₈, Na₂ P₈ O₂₁, K.sub. 4 P₆ O₁₇ and the like. The metallic phosphate condensation catalysts having an acyclic structure used herein should be capable of being transformed into a cyclic structure under the reaction conditions. The preferred metallic phosphate condensation catalysts for use in this invention include Group IA metal metaphosphates, Group IA meal dihydrogen orthophosphates and Group IA metal dihydrogen pyrophosphates, more preferably Na₃ P₃ O₉, NaH₂ PO₄ and Na₂ H₂ P₂ O₇. Other suitable metallic phosphate condensation catalysts having a cyclic structure or an acyclic structure capable of being transformed into a cyclic structure during the process which are embraced within the scope of this invention are disclosed by Van Wazer, J. R., Phosphorus and Its Compounds, Vol. 1, Interscience Publishers, Inc., New York (1958).

As indicated above, metallic phosphate condensation catalysts having an acyclic structure are suitable for use in the process of this invention provided that the acyclic structure is transformed into a cyclic structure during the reaction. Suitable catalysts for use in the process of this invention include metallic phosphates having a cyclic structure, metallic phosphates having an acyclic structure which are transformed into a cyclic structure during the reaction and mixtures of metallic phosphates having a cyclic structure with metallic phosphates having an acyclic structure which may or may not transform into a cyclic structure during the reaction it is recognized that any combination of metallic phosphates may be used in the process of this invention provided at least one metallic phosphate having a cyclic structure is present during the reaction. It is also recognized that metallic phosphates having a cyclic structure can be formed under reaction conditions from any combination of metallic phosphates having an acyclic structure and/or cyclic structure or other reactants in the process.

The metallic phosphate condensation catalysts can be prepared by conventional methods known in the art. Sodium is believed to be one of a small group of cations effective for stabilizing six-membered cyclic metaphosphates at their temperatures of fusion (about 625° C.) without decomposition to linear and/or other phosphates including mixtures. The formation of cyclic and acyclic metallic phosphate structures appears to depend on the cation ionic size, the coordination number of the cation and the ionic or covalent nature of the metal-oxygen bond.

The level of activity of the metallic phosphate catalyst of the invention is that level which of itself makes the catalyst at least as active in the condensation of amines as, for example, is phosphoric acid on an equivalent basis. Preferably, supported metallic phosphate condensation catalysts should have a surface area greater than about 70 m² /gm to as high as about 260 m² /gm or greater depending upon which metal oxide described below that is employed. In the case of titanium oxides, the surface area should be greater than about 140 m² / gm to as high as about 260 m² /gm, more preferably, greater than about 160 m^(2/) gm to as high as about 260 m² /gm, determined according to the single point N₂ method. In the case of zirconia oxides, the surface area should be greater than about 70 m² /gm to as high as about 150 m² /gm, more preferably, greater than about 90 m² /gm to as high as about 135 m² /gm, determined according to the single point N₂ method. It is appreciated that the metal oxides described below which can be used in association with the metallic phosphate condensation catalyst and the performance moderators described below can affect the surface area of the metallic phosphate condensation catalyst. While surface areas described above may be preferred, for purposes of this invention, the surface area of the metallic phosphate condensation catalyst should be sufficient to contribute to product selectivity, catalytic activity and/or mechanical or dimensional strength of the catalyst.

The metallic phosphate condensation catalysts useful in this invention can be associated with one or more metal oxides. Preferred metal oxides are amphoteric or slightly acidic or slightly basic. Illustrative of such metal oxides which may be utilized in association with the metallic phosphate condensation catalyst include, for example, one or more of the following: Group IA metal oxides, Group IIA metal oxides, Group IIIB metal oxides (including lanthanides and actinides), Group VB metal oxides, Group VIB metal oxides, Group VIIB metal oxides, Group VIII metal oxides, Group IB metal oxides, Group IIB metal oxides, Group IIIA metal oxides, Group IVA metal oxides, Group VA metal oxides, Group VIA metal oxides and Group IVB metal oxides or mixtures thereof. Preferred metal oxides which may be utilized in association with the metallic phosphate condensation catalyst include, for example, one or more oxides of beryllium, scandium, yttrium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, titanium, zirconium, hafnium, vanadium, niobium, tantalum, tungsten, iron, cobalt, zinc, silver, aluminum, gallium, indium, silicon, germanium, tin, lead, arsenic, antimony and bismuth.

Group IVA and IVB metal oxides such as silica, titanium dioxide and zirconium dioxide are preferred for use in this invention. For mixed metal oxides in which at least one of the metals is titanium, suitable metals in association with titanium may include, for example, one or more of the following: Group IIIB metals such as scandium, yttrium and lanthanum including the lanthanides, Group VB metals such as niobium and tantalum, Group VIB metals such as chromium, molybdenum and tungsten, Group VIII metals such as iron, cobalt and nickel, Group IIB metals such as zinc and cadmium, Group IIIA metals such as boron, aluminum, gallium and indium, Group IVA metals such as silicon, germanium, tin and lead, Group VA metals such as arsenic, antimony and bismuth, and Group IVB metals such as zirconium and hafnium. For mixed metal oxides in which at least one of the metals is zirconium, suitable metals in association with zirconium may include, for example, one or more of the following: Group IVA metals such as silicon, germanium, tin and lead, Group VB metals such as niobium and tantalum, and Group VIB metals such as chromium, molybdenum and tungsten. The virtue of these metal oxides is that they demonstrate higher mechanical strength than the metallic phosphate component per se and can contribute to product selectivity and catalytic activity.

Illustrative of mixed metal oxides which may be used in association with the metallic phosphate catalyst include, for example, TiO₂ --SiO₂, TiO₂ --Al₂ O₃, TiO₂ --CdO, TiO₂ --Bi₂ O₃, TiO₂ --Sb₂ O₅, TiO₂ --SnO₂, TiO₂ --ZrO₂, TiO₂ --BeO, TiO₂ --MgO, TiO₂ --CaO, TiO₂ --SrO, TiO₂ --ZnO, TiO₂ --Ga₂ O₃, TiO₂ --Y₂ O₃, TiO₂ La₂ O₃, TiO₂ --MoO₃, TiO₂ --Mn₂ O₃, TiO₂ --Fe₂ O₃, TiO₂ --Co₃ O₄, TiO₂ --WO₃, TiO₂ --V₂ O₅, TiO₂ --Cr₂ O₃, TiO₂ --ThO₂, TiO₂ --Na₂ O, TiO₂ --BaO, TiO₂ --CaO, TiO₂ --HfO₂, TiO₂ --Li₂ O, TiO₂ --Nb₂ O₅ , TiO₂ --Ta₂ O₅, TiO₂ --Gd₂ O₃, TiO₂ --Lu₂ O₃, TiO₂ --Yb₂ O₃, TiO₂ --CeO₂, TiO₂ --Sc₂ O₃, TiO₂ --PbO, TiO₂ --NiO, TiO₂ --CuO, TiO₂ --CoO, TiO₂ --B₂ O₃, ZrO₂ --SiO₂, ZrO₂ --Al₂ O₃, ZrO₂ --SnO, ZrO₂ --PbO, ZrO₂ --Nb₂ O₅, ZrO₂ --Ta₂ O₅, ZrO₂ --Cr₂ O₃, ZrO₂ --MoO₃, ZrO₂ --WO₃, ZrO₂ -TiO₂, ZrO₂ --HfO₂, TiO₂ --SiO₂ --Al₂ O₃, TiO₂ --SiO₂ --ZnO, TiO₂ --SiO₂ --ZrO₂, TiO₂ --SiO₂ --CuO, TiO₂ --SiO₂ --MgO, TiO₂ --SiO₂ --Fe₂ O₃, TiO₂ --SiO₂ --B₂ O₃, TiO₂ --SiO₂ --WO₃, TiO₂ --SiO₂ --Na₂ O, TiO₂ --SiO₂ --MgO, TiO₂ --SiO₂ --La₂ O₃, TiO₂ --SiO₂ --Nb₂ O₅, TiO₂ --SiO₂ --Mn₂ O₃, TiO₂ --SiO₂ --Co₃ O₄, TiO₂ --SiO₂ --NiO, TiO₂ SiO₂ --PbO, TiO₂ --SiO₂ --Bi₂ O₃, TiO₂ --Al₂ O₃ --ZnO, TiO₂ --Al₂ O₃ --ZrO₂, TiO₂ --Al₂ O₃ --Fe₂ O₃, TiO₂ --Al₂ O₃ --WO₃, TiO₂ --Al₂ O₃ --La₂ O₃, TiO₂ --Al.sub. 2 O₃ --Co₃ O₄, ZrO₂ --SiO₂ --Al₂ O₃, ZrO₂ --SiO₂ --SnO, ZrO₂ --SiO₂ --Nb₂ O₅, ZrO₂ --SiO₂ --WO₃, ZrO₂ --SiO₂ --TiO₂, ZrO₂ --SiO₂ --MoO₃, ZrO₂ --SiO₂ --HfO₂, ZrO₂ --SiO₂ --Ta₂ O₅, ZrO₂ --Al₂ O₃ --SiO₂, ZrO₂ --Al₂ O₃ --PbO, ZrO₂ --Al₂ O₃ --NbO₂ O₅, ZrO₂ --Al₂ O₃ --WO₃, ZrO₂ --Al₂ O₃ --TiO₂, ZrO₂ --Al₂ O₃ --MoO₃, ZrO₂ --HfO₂ --Al₂ O₃, ZrO₂ --HfO₂ --TiO₂, and the like. Other suitable mixed metal oxide catalysts embraced within the scope of this invention are disclosed by Tanabe et al., Bulletin of the Chemical Society of Japan, Vol. 47(5), pp. 1064-1066 (1974).

The metal oxides described herein which can be used in association with the metallic phosphate catalyst may contribute to product selectivity and/or catalytic activity of the reaction and/or stability of the catalyst. The catalyst structure can comprise from about 0 to about 90 percent or greater by weight of the metal oxide, preferably from about 0 to about 75 percent by weight of the metal oxide, and more preferably from about 0 to about 50 percent by weight of the metal oxide, the remainder being the weight of the metallic phosphate catalyst. For mixed metal oxides containing titania, higher concentrations of titania can provide very desirable product selectivities including acyclic to cyclic selectivities and linear to branched selectivities of higher polyalkylene polyamine products. As discussed hereinafter, the metallic phosphate condensation catalyst of this invention may also contain support(s), binding agent(s) or other additives to stabilize or otherwise help in the manufacture of the catalyst.

Though the metallic phosphate condensation catalyst of the invention provides sufficient activity to effect the condensation reaction, certain combinations of reactants and/or product formation may be benefited by treating the catalyst with a catalyst moderator, hereinafter termed "performance moderator. " Catalyst moderators are widely used to control the performance of catalysts in areas of selectivity to certain products and the repression of a catalyst's proclivity to generate a broad range of reaction products. A range of suitable materials may impact the metallic phosphate condensation catalysts of this invention in the variety of reaction products. The performance moderator may be any material which impacts the metallic phosphate condensation catalyst's selection of reaction products or which changes the proportion of any one or more of the reaction products which the metallic phosphate condensation catalyst generates at comparable processing conditions. In addition to contributing to product selectivity, the performance moderator may be any material which contributes to catalytic activity and/or catalyst stability (mechanical or dimensional strength).

An illustrative performance moderator is a mineral acid or a compound derived from a mineral acid. Suitable for use as performance moderators are one or more phosphoric acid or a salt of phosphoric acid, hydrogen fluoride, hydrofluoric acid or a fluoride salt, sulfuric acid or a salt of sulfuric acid, and the like. The moderator may also be organic esters of phosphoric acid or a salt of phosphoric acid, hydrogen fluoride organic complexes, hydrofluoric acid organic complexes or a fluoride salt organic complexes, organic esters of sulfuric acid or a salt of sulfuric acid, and the like. Suitable salts of phosphoric acid include sodium dihydrogen phosphate, disodium hydrogen phosphate, sodium phosphate and the like. Other illustrative performance moderators include the metal oxides described above which can be used in association with the metallic phosphate condensation catalyst and also metallic phosphates which may or may not have a cyclic structure. Certain of these metallic phosphate performance moderators may also be effective as catalysts for use in this invention.

The metal oxides described hereinabove which can be used in association with the metallic phosphate catalyst can also be used as performance moderators in accordance with this invention. The metal oxides can contribute to product selectivity, catalytic activity and/or catalyst stability (mechanical strength).

As indicated above, other performance moderators which can be used in accordance with this invention include metallic phosphates which may or may not have a cyclic structure. Corresponding metallic metaphosphimates, metallic phosphoramidates and metallic amido- and imidophosphates of the above may also be used as performance moderators in accordance with this invention. Such metallic phosphates can contribute to product selectivity, catalytic activity and/or catalyst stability (mechanical strength).

Other performance moderators which can be used in accordance with this invention include metallic polyphosphates which may or may not have a condensed structure. Suitable metallic polyphosphates having a condensed structure are disclosed in U.S. patent application Ser. No. (390,709), filed on an even date herewith and incorporated herein by reference. Corresponding metallic metaphosphimates, metallic phosphoramidates and metallic amido- and imidophosphates of the above may also be used as performance moderators in accordance with this invention. Illustrative metallic polyphosphates having a condensed structure include many of the metallic phosphates described above.

Group VIB metal-containing substances may be used as performance moderators in accordance with this invention. Suitable Group VIB metal-containing substances are disclosed in U.S. patent application Ser. No. (390,708), filed on an even date herewith and incorporated herein by reference. Illustrative of Group VIB metal-containing performance moderators include, for example, one or more oxides of tungsten, chromium, molybdenum or mixtures thereof.

A variety of conventional phosphorus-containing substances may be suitable for use as performance moderators in this invention. The conventional substances should be capable of functioning as a performance moderator. Illustrative of conventional phosphorus containing substances may include, for example, those disclosed in U.S. Pat. No 4,036,881, U.S. Pat. No. 4,806,517, U.S. Pat. No. 4,617,418, U.S. Pat. No. 4,720,588, U.S. Pat. No. 4,394,524, U.S. Pat. No. 4,540,822, U.S. Pat. No. 4,588,842, U.S. Pat. No. 4,605,770, U.S. Pat. No. 4,683,335, U.S. Pat. No. 4,316,841, U.S. Pat. No. 4,463,193, U.S. Pat. No. 4,503,253, U.S. Pat. No. 4,560,798 and U.S. Pat. No. 4,578,517.

Suitable conventional phosphorus-containing substances which may be employed as performance moderators in this invention include acidic metal phosphates, phosphoric acid compounds and their anhydrides, phosphorous acid compounds and their anhydrides, alkyl or aryl phosphate esters, alkyl or aryl phosphite esters, alkyl or aryl substituted phosphorous acids and phosphoric acids, alkali metal monosalts of phosphoric acid, the thioanalogs of the foregoing, and mixtures of any of the above.

The amount of the performance moderator of the mineral acid type used with the metallic phosphate catalyst of the invention is not narrowly critical. Generally, the amount does not exceed 25 weight percent of the weight of the catalyst. As a rule, it is desirable to use at least 0.01 weight percent of the weight of the catalyst. Preferably, the amount of performance moderator, when used, will range from about 0.2 to about 10 weight percent of the weight of the catalyst. Most preferably, the amount of performance moderator, when used, will range from about 0.5 to about 5 weight percent of the weight of the catalyst.

The amount of performance moderator other than the mineral acid type used with the metallic phosphate catalyst is not narrowly critical. Generally, the amount does not exceed 90 weight percent of the weight of the catalyst. The amount of performance moderator can range from about 0 to about 90 or greater weight percent of the weight of the catalyst, preferably from about 0 to about 75 weight percent of the weight of the catalyst, and more preferably from about 0 to about 50 weight percent of the weight of the catalyst. Most preferably, the amount of performance moderator, when used, will range from about 0.5 to about 25 weight percent of the weight of the catalyst.

This invention also embraces the use of vicinal di(hetero)alkylene organometalates in the preparation of amines. Suitable vicinal di(hetero)alkylene organometalates are disclosed in U.S. patent application Ser. No. 390,828, filed on an even date herewith and incorporated herein by reference.

The performance moderator can be provided to the metallic phosphate catalyst by conventional procedures known in the art. For example, the performance moderator can be provided to the catalyst by impregnating particles or monolithic structures comprising the metallic phosphate catalyst with liquid comprising the performance moderator. This is a well known procedure in the art for incorporating additives to a solid support material. The metallic phosphate catalyst of the invention may be utilized as solid powders or as fused, bonded or compressed solid pellets, or larger structures in association with the one or more metal oxides, or as coated, fused, bonded or compressed solid pellets, or larger structures, composited with one or more support materials, in association with one or more metal oxides. These solid structures may be treated with the performance moderator by mixing a liquid body of the performance moderator with the solid structure. For example, the metallic phosphate catalyst solids may be slurried in the performance moderator, drained, washed and suctioned to remove excess performance moderator, and then dried with heat to remove any volatiles accompanying the performance moderator. The drying temperature chosen will depend on the nature of the volatiles to be removed. Usually, the time/temperature for effecting drying will be below the conditions for effecting dehydration to remove bound water from the metal oxide in association with the metallic phosphate catalyst. Normally the drying temperature will be greater than about 120° C. and below about 600° C. depending on the thermal stability of the catalyst. The drying time will generally go down as the drying temperature rises and vice versus, and may extend from 5 seconds to about 24 hours.

Alternatively, the performance moderator can be provided to the catalyst at the time of preparing the metallic phosphate catalyst in association with one or more metal oxides. For example, one or more metal oxides may be condensed from their respective hydrolyzable monomers to the desired oxides to form oxide powders which can thereafter be blended and compressed with the metallic phosphate to form pellets and larger structures of the metal oxide-containing condensation catalyst of this invention. The one or more metal oxides which can be used in association with the metallic phosphate catalyst in accordance with this invention can be provided from metal salts which can be heated to form the metal oxide. It is appreciated that the performance moderator can be incorporated into the molecular bonding configuration of the metal oxide-containing condensation catalyst by conventional procedures known in the art.

The metallic phosphate condensation catalysts in association with one or more metal oxides prior to the optional treatment of the performance moderator may be prepared in a wide variety of ways. For example, one or more metal oxides may be provided as a partial condensate on a support, such as a silica or alpha, beta or gamma alumina, silicon carbide, and the like, and then condensed by heating to effect polymerization to the desired oxide form. The metal oxide(s) may be condensed from hydrolyzable monomers to the desired oxide, indeed, to form an oxide powder which can thereafter be compressed in the presence of a metallic phosphate to form pellets and larger structures of the metal oxide-containing condensation catalyst of the invention. A blend of the powder and metallic phosphate can be made into a shapeable paste which can be extruded and cut into pellets according to conventional procedures. The extrudate may thereafter be fired to cure the metallic phosphate and fix the structure. The cut extrudate may be blended with a support material such as those characterized above, and the blend fired to fuse the metal oxide-containing catalyst to the support.

In a preferred embodiment of this invention, a high surface area silica or titania can be slurried with an aqueous solution of sodium dihydrogen phosphate, disodium dihydrogen pyrophosphate or sodium trimetaphosphate, extruded, and calcined at a temperature of about 400° C.

A preferred catalyst structure comprises sodium dihydrogen phosphate, disodium dihydrogen pyrophosphate or sodium trimetaphosphate in association with a Group IVA or IVB metal oxide having a surface area of at least a 140 m² /gm which may or may not be bonded to a support material. The term "support," as used herein and in the claims, means a solid structure which does not adversely affect the catalytic properties of the catalyst and is at least as stable as the catalyst to the reaction medium. The support can function as an amine condensation catalyst independent of the metallic phosphate having a cyclic structure, although it may have lower catalytic activity to the reaction. The support may act in concert with the catalyst to moderate the reaction. Some supports may contribute to the selectivity of the reaction. The catalyst structure can comprise from about 2 to about 60 percent by weight or greater of the support, more preferably from about 10 to about 50 percent by weight of the support, the remainder being the weight of the metal oxide(s) and metallic phosphate. Included in the weight of the support is the weight of any binding agent such as phosphates, sulfates, silicates, fluorides, and the like, and any other additive provided to stabilize or otherwise help in the manufacture of the catalyst. The support may be particles as large or larger than the catalyst component and "glued" to the catalytic metallic phosphate and/or metal oxide by virtue of a binding medium.

The support may constitute a separate phase in the process of extruding the catalytic structure. In this embodiment, the support forming material, preferably as a paste is blended with a paste of the metallic phosphate and one or more metal oxides or a partial condensate thereof. The paste may comprise the oxide forms of the support and the metallic phosphate, each blended with water, and/or binding agents. The extrudate of the blend is passed through a multiorificed die and chopped into pellets of the desired sizes. The particles may be doughnut shaped, spherical, and the like. Then the particles are calcined to dry them and complete any condensation reaction in the support and/or the metal oxide-containing condensation catalyst.

The use of supports for the metallic phosphate condensation catalyst provides a number of significant advantages. It has been determined that some of the metallic phosphates are not as stable in the amines reaction media when utilized over an extended period of time. When the reaction is effected as a batch reaction, this matter is not a problem. However, when the reaction is effected with the metallic phosphate catalyst as part of a fixed bed in a tubular reactor, the preferred procedure for carrying out the invention, it is desirable to have the catalyst be more stable. When the catalyst is combined with the support, the catalyst has greater stability for the reaction medium, and therefore, it is better able to be used in a fixed bed of a continuous reactor. The supported catalysts suffer from none of the leaching problems that the catalyst per se may have or the problems that are associated with the prior art catalysts, such as acidic phosphorus compounds on silica.

The reactants used in the condensation process of the invention may be ammonia or organic compound containing --NH-- and any compound possessing an alcoholic hydroxyl group, subject to the following: the intramolecular condensation of an amino compound produces an amine having a lower molecular weight, and the intermolecular condensation of an amino compound with one or more of another amino compound or a compound containing an alcoholic hydroxyl group produces an amine having a lower, same or higher molecular weight than the reactants.

Illustrative of suitable reactants in effecting the process of the invention, include by way of example:

Ammonia

MEA--monoethanolamine

EDA--ethylenediamine

MeEDA--methylethylenediamine

EtEDA--ethylethylenediamine

AEEA--N-(2-aminoethyl)ethanolamine

HEP--N-(2-hydroxyethyl)piperazine

DETA--diethylenetriamine

AEP--N-(2-aminoethyl)piperazine

TAEA--trisaminoethylamine

TETA--triethylenetetramine

TEPA--tetraethylenepentamine

PEHA--pentaethylenehexamine

TETA Isomers

TAEA--trisaminoethylamine

TETA--triethylenetetramine

DPE--dipiperazinoethane

DAEP--diaminoethylpiperazine

PEEDA--piperazinoethylethylenediamine

TEPA Isomers

AETAEA--aminoethyltrisaminoethylamine

TEPA--tetraethylenepentamine

AEDPE--aminoethyldipiperazinoethane

AEPEEDA--aminoethylpiperazinoethylethylenediamine

iAEPEEDA--isoaminoethylpiperazinoethylethylenediamine

AEDAEP--aminoethyldiaminoethylpiperazine

BPEA--bispiperazinoethylamine

The foregoing also can represent the products of the reaction. For example, ammonia and MEA are frequently employed to produce EDA along with a variety of other amines, most of which are set forth above.

Glycol compounds can also be employed in the preparation of amines in accordance with this invention. For purposes of this invention, glycol compounds embrace diols and polyols. Illustrative of suitable glycol compounds include alkylene glycols such as ethylene glycol, propylene glycol, 1,3-propane diol or mixtures thereof.

The process may be effected in the liquid or vapor or supercritical liquid states or mixtures thereof though the actual reaction is believed to occur on the catalyst s solid surface in the absorbed state. In this context, the vapor phase reaction is intended to refer to the general vapor state of the reactants. Though the reaction conditions may range from subatmospheric to superatmospheric conditions, it is desirable to run the reaction from about 50 psig to about 3,000 psig, preferably from about 200 psig to about 2,000 psig.

The temperature of the reaction may be as low as about 125° C. to about 400° C. Preferably, the reaction temperature ranges from about 150° C. to about 350° C., and most preferably from about 225° C. to about 325° C.

The reaction may be effected by the incremental addition of one of the reactants to the other or by the joint addition of the reactants to the catalyst. The preferred process effects the reaction in a continuous manner over a fixed bed of the metallic phosphate catalyst in a tubular reactor. However, the reaction may be carried out by slurrying the catalyst in the reactants or in a batch mode in an autoclave. An inert such as nitrogen, methane and the like can be used in the reaction process

The preferred process involves the formation of alkyleneamines from the intermolecular condensation of alkanolamines and alkyleneamines or the intramolecular condensation of alkyleneamines or alkanolamines. Illustrative of such reactions are the following reactant combinations:

    ______________________________________                                         REACTANT   REACTANT   PRODUCTS                                                 ______________________________________                                         Ammonia    Methanol   Monomethylamine                                                                Dimethylamine                                                                  Trimethylamine                                           Ammonia    MEA        EDA, DETA, AEEA,                                                               TETA, TEPA, PIP                                          Ammonia    AEEA       DETA, PIP                                                MEA, Ammonia                                                                              EDA        EDA, AEEA, HEP,                                                                DETA, AEP, TETA,                                                               TEPA, PEHA,                                                                    TETA Isomers:                                                                  TAEA, TETA, DAEP,                                                              PEEDA, DPE                                                                     TEPA, TEPA Isomers:                                                            AETAEA, AEPEEDA.                                                               AEDAEP, AEDPE, BPEA                                      MEA        EDA        AEEA, HEP, DETA,                                                               AEP, TETA, TEPA,                                                               PEHA, TETA Isomers:                                                            TAEA, TETA, DAEP,                                                              PEEDA, DPE                                                                     TEPA, TEPA Isomers:                                                            AETAEA, AEPEEDA,                                                               AEDAEP, AEDPE, BPEA                                      EDA        AEEA       HEP, AEP, TETA,                                                                TEPA, PEHA,                                                                    TETA Isomers:                                                                  TAEA, TETA, DAEP,                                                              PEEDA, DPE                                                                     TEPA, TEPA Isomers:                                                            AETAEA, AEPEEDA,                                                               AEDAEP, AEDPE, BPEA                                      DETA       AEEA       TEPA Isomers,                                                                  AEP                                                      EDA        EDA        DETA, TETA AND                                                                 TEPA Isomers                                             ______________________________________                                    

The process of the invention provides the ability to generate the manufacture of desirable higher polyalkylene polyamine products such as TETA, TEPA and PEHA without generating large amounts of cyclic alkylenepolyamine products such as PIP, AEP and HEP. The alkyleneamines producers composition of this invention has a TETA+TAEA to PIP+AEP+PEEDA+DAEP+DPE weight ratio of greater than about 0.5, a TETA to TAEA weight ratio of greater than about 2.0 and a TEPA to AETAEA weight ratio of greater than about 2.0.

The process of this invention provides the potential to control congener distribution, linear to cyclic selectivity and linear to branched selectivity of the higher polyalkylene polyamines.

It is appreciated that the metallic phosphate condensation catalysts of this invention may also be useful in the production of alkylamines. For example, an alcohol and at least one of ammonia, a primary amine, a secondary amine or a tertiary amine may be contacted in the presence of a metallic phosphate condensation catalyst having a cyclic structure or an acyclic structure which is transformed into a cyclic structure during the process under conditions effective to produce alkylamines.

This invention is further illustrated by certain of the following examples:

EXAMPLES

In the examples set forth in the tables below, the catalyst of choice was placed in one of three tubular reactors, each having an outside diameter of 1 inch and an overall length of 24 inches. The catalyst portion of the reactor was sufficient for accommodating 100 cubic centimeters of catalyst. The reactor was made of 316 stainless steel. As used herein, ABl refers to a material obtained from Norton Company, Akron, Ohio, which is a mixture of sodium trimetaphosphate and sodium tripolyphosphate. As used in the tables below, acyclic (N4)/cyclic (<=N4) refers to the weight ratio of TETA+TAEA to PIP+AEP+PEEDA+DAEP+DPE. The catalysts employed are identified as follows:

    ______________________________________                                         Designation                                                                               Composition   Physical Properties                                   ______________________________________                                         A          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/sodium                                                                             inch cylindrical                                                 trimetaphosphate;                                                                            extrudates; Catalyst                                             Ti:P atom ratio =                                                                            surface area: 133.3                                              5.7:1         m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.344 cc/gm;                                                         Pore area: 83.5                                                                m.sup.2 /gm; Bulk                                                              density: 1.55 gm/cc.                                  B          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/sodium                                                                             inch cylindrical                                                 tripolyphosphate;                                                                            extrudates; Catalyst                                             Ti:P atom ratio =                                                                            surface area: 80.3                                               5.7:1         m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.236 cc/gm;                                                         Pore area: 54.2                                                                m.sup.2 /gm; Bulk                                                              density: 1.72 gm/cc.                                  C          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1;                                                                               inch cylindrical                                                 Ti:P atom ratio =                                                                            extrudates; Catalyst                                             5.7:1         surface area: 115.0                                                            m.sup.2 /gm; Pore                                                              volume N.sub.2 : 0.429                                                         cc/gm; Pore area:                                                              87.4 m.sup.2 /gm; Bulk                                                         density: 1.39 gm/cc.                                  D          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/sodium                                                                             inch cylindrical                                                 pyrophosphate;                                                                               extrudates; Catalyst                                             Ti:P atom ratio =                                                                            surface area: 78.6                                               5.7:1         m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.339 cc/gm;                                                         Pore area: 72.1                                                                m.sup.2 /gm; Bulk                                                              density: 1.59 gm/cc.                                  E          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 boric acid (2 extrudates; Catalyst                                             wt. %)        surface area: 97.1                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.440 cc/gm;                                                         Pore area: 84.2                                                                m.sup.2 /gm; Bulk                                                              density: 1.32 gm/cc.                                  F          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 ammonium tetra-                                                                              extrudates; Catalyst                                             fluoroborate  surface area: 39.6                                               (2 wt. %)     m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.442 cc/gm;                                                         Pore area: 66.7                                                                m.sup.2 /gm; Bulk                                                              density: 1.34 gm/cc.                                  G          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 sodium tetra- extrudates; Catalyst                                             fluoroborate  surface area: 44.1                                               (8 wt. %)     m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.432 cc/gm;                                                         Pore area: 69.1                                                                m.sup.2 /gm; Bulk                                                              density: 1.35 gm/cc.                                  H          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 sodium tetra- extrudates; Catalyst                                             fluoroborate  surface area: 23.0                                               (8 wt. %)     m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.373 cc/gm;                                                         Pore area: 36.6                                                                m.sup.2 /gm; Bulk                                                              density: 1.57 gm/cc.                                  I          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 sodium meta-  extrudates; Catalyst                                             tungstate     surface area: 91.3                                               (1 wt. %)     m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.414 cc/gm;                                                         Pore area: 75.7                                                                m.sup.2 /gm; Bulk                                                              density: 1.40 gm/cc                                   J          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 sodium meta-  extrudates; Catalyst                                             tungstate     surface area: 101.2                                              (2 wt. %)     m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.442 cc/gm;                                                         Pore area: 94.2                                                                m.sup.2 /gm; Bulk                                                              density: 1.38 gm/cc.                                  K          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 sodium meta-  extrudates; Catalyst                                             tungstate     surface area: 100.2                                              (4 wt. %)     m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.429 cc/gm;                                                         Pore area: 90.0                                                                m.sup.2 /gm; Bulk                                                              density: 1.43 gm/cc.                                  L          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 ammonium meta-                                                                               extrudates; Catalyst                                             tungstate     surface area: 97.9                                               (2 wt. % as WO.sub.3)                                                                        m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.431 cc/gm;                                                         Pore area: 79.4                                                                m.sup.2 /gm; Bulk                                                              density: 1.43 gm/cc.                                  M          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 ammonium meta-                                                                               extrudates; Catalyst                                             tungstate     surface area: 91.8                                               (4 wt. % as WO.sub.3)                                                                        m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.402 cc/gm;                                                         Pore area: 69.2                                                                m.sup.2 /gm; Bulk                                                              density: 1.51 gm/cc.                                  N          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 ammonium meta-                                                                               extrudates; Catalyst                                             tungstate     surface area: 78.1                                               (8 wt. % as WO.sub.3)                                                                        m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.403 cc/gm;                                                         Pore area: 74.0                                                                m.sup.2 /gm; Bulk                                                              density: 1.47 gm/cc.                                  O          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 lanthanum oxide                                                                              extrudates; Catalyst                                             (2 wt. %)     surface area: 102.8                                                            m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.409 cc/gm;                                                         Pore area: 65.3                                                                m.sup.2 /gm; Bulk                                                              density: 1.49 gm/cc.                                  P          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 lanthanum oxide                                                                              extrudates; Catalyst                                             (4 wt. %)     surface area: 102.6                                                            m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.418 cc/gm;                                                         Pore area: 85.4                                                                m.sup.2 /gm; Bulk                                                              density: 1.41 gm/cc.                                  Q          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 niobium oxide extrudates; Catalyst                                             (2 wt. %)     surface area: 102.8                                                            m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.435 cc/gm;                                                         Pore area: 85.5                                                                m.sup.2 /gm; Bulk                                                              density: 1.35 gm/cc.                                  R          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 sodium bicarbonate                                                                           extrudates; Catalyst                                             (2 wt. %)     surface area: 99.5                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.417 cc/gm;                                                         Pore area: 76.4                                                                m.sup.2 /gm; Bulk                                                              density: 1.41 gm/cc.                                  S          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 vanadium oxide                                                                               extrudates; Catalyst                                             (2 wt. %)     surface area: 88.7                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.411 cc/gm;                                                         Pore area: 63.9                                                                m.sup.2 /gm; Bulk                                                              density: 1.44 gm/cc.                                  T          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/SiO.sub.2 /                                                                        inch cylindrical                                                 Al.sub.2 O.sub.3 /sodium                                                                     extrudates; Catalyst                                             trimetaphosphate                                                                             surface area: 129.9                                              (10 wt. %)    m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.321 cc/gm;                                                         Pore area: 163                                                                 m.sup.2 /gm; Bulk                                                              density: 1.59 gm/cc.                                  U          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/SiO.sub.2 /                                                                        inch cylindrical                                                 B.sub.2 O.sub.3 /sodium                                                                      extrudates; Catalyst                                             trimetaphosphate                                                                             surface area: 159.5                                              (10 wt %)     m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.312 cc/gm;                                                         Pore area: 129.8                                                               m.sup.2 /gm, Bulk                                                              density: 1.54 gm/cc.                                  V          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/SiO.sub.2 /                                                                        inch cylindrical                                                 sodium trimeta-                                                                              extrudates; Catalyst                                             phosphate     surface area: 136.5                                              (10 wt %)     m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.399 cc/gm;                                                         Pore area: 162.5                                                               m.sup.2 /gm; Bulk                                                              density: 1.48 gm/cc.                                  W          Titanium dioxide/                                                                            Particle size: 1/16                                              AB1           inch cylindrical                                                               extrudates; Catalyst                                                           surface area: 4.40                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.184 cc/gm;                                                         Pore area: 19.2                                                                m.sup.2 /gm; Bulk                                                              density: 2.10 gm/cc.                                  X          Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1 inch cylindrical                                                               extrudates; Catalyst                                                           surface area: 102.0                                                            m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.406 cc/gm;                                                         Pore area: 68.6                                                                m.sup.2 /gm; Bulk                                                              density: 1.43 gm/cc.                                  Y          Maqnesium oxide/                                                                             Particle size: 1/16                                              AB1           inch cylindrical                                                               extrudates; Catalyst                                                           surface area: 18.1                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.298 cc/gm;                                                         Pore area: 52.9                                                                m.sup.2 /gm; Bulk                                                              density: 1.78 gm/cc.                                  Z          Silicon dioxide/                                                                             Particle size: 1/16                                              AB1           inch cylindrical                                                               extrudates; Catalyst                                                           surface area: 33.7                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.496 cc/gm;                                                         Pore area: 81.0                                                                m.sup.2 /gm; Bulk                                                              density: 1.06 gm/cc.                                  AA         Aluminum oxide/                                                                              Particle size: 1/16                                              lanthanum meta-                                                                              inch cylindrical                                                 phosphate     extrudates; Catalyst                                                           surface area: 86.0                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.327 cc/gm;                                                         Pore area: 129.5                                                               m.sup.2 /gm; Bulk                                                              density: 1.57 gm/cc.                                  BB         Silicon dioxide/                                                                             Particle size: 1/16                                              lanthanum meta-                                                                              inch cylindrical                                                 phosphate     extrudates; Catalyst                                                           surface area: 38.7                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.656 cc/gm;                                                         Pore area: 90.5                                                                m.sup.2 /gm; Bulk                                                              density: 0.99 gm/cc.                                  CC         Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/ZnO                                                                            inch cylindrical                                                 (2 wt. %)     extrudates; Catalyst                                                           surface area: 90.4                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.427 cc/gm;                                                         Pore area: 74.5                                                                m.sup.2 /gm; Bulk                                                              density: 1.49 gm/cc.                                  DD         Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/ZnO                                                                            inch cylindrical                                                 (4 wt. %)     extrudates; Catalyst                                                           surface area: 78.3                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.412 cc/gm;                                                         Pore area: 75.1                                                                m.sup. 2 /gm; Bulk                                                             density: 1.42 gm/cc.                                  EE         Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 Nb.sub.2 O.sub.5                                                                             extrudates; Catalyst                                             (4 wt. %)     surface area: 102.2                                                            m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.407 cc/gm;                                                         Pore area: 75.4                                                                m.sup.2 /gm; Bulk                                                              density: 1.44 gm/cc.                                  FF         Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/AB1/                                                                               inch cylindrical                                                 NaBF.sub.4 (8 wt. %)                                                                         extrudates; Catalyst                                                           surface area: 22.5                                                             m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.421 cc/gm;                                                         Pore area: 55.8                                                                m.sup.2 /gm; Bulk                                                              density: 1.38 gm/cc.                                  GG         Titanium dioxide                                                                             Particle size:                                                   (anatase)/sodium                                                                             1/16 inch cylindri-                                              dihydrogen phos-                                                                             cal extrudates;                                                  phate; Ti:P atom                                                                             Catalyst surface                                                 ratio = 5.7:1 area: 117.1                                                                    m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.321 cc/gm;                                                         Pore area: 85.7                                                                m.sup.2 /gm; Bulk                                                              density: 1.64                                                                  gm/cc.                                                HH         Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/disodium                                                                           inch cylindrical                                                 dihydrogen pyro-                                                                             extrudates; Cata-                                                phosphate; Ti:P                                                                              lyst surface area:                                               atom ratio =  133.5 m.sup.2 /gm; Pore                                          5.7:1         N.sub.2 : 0.291 cc/gm;                                                         Pore area: 89.6                                                                m.sup.2 /gm; Bulk                                                              denisity: 1.66                                                                 gm/cc.                                                II         Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/disodium                                                                           inch cylindrical                                                 hydrogen phosphate;                                                                          extrudates; Cata-                                                Ti:P atom ratio =                                                                            lyst surface area:                                               5.7:1         117/4 m.sup.2 /gm; Pore                                                        volume N.sub.2 : 0.346                                                         cc/gm; Pore area                                                               86.5 m.sup.2 /gm; Bulk                                                         density: 1.53 gm/cc.                                  JJ         Titanium dioxide                                                                             Particle size: 1/16                                              (anatase)/sodium                                                                             inch cylindrical                                                 phosphate; Ti:P                                                                              extrudates; Catalyst                                             atom ratio =  surface area: 88.4                                               5.7:1         m.sup.2 /gm; Pore volume                                                       N.sub.2 : 0.365 cc/gm;                                                         Pore area: 76.90                                                               m.sup.2 /gm; Bulk                                                              density: 1.48 gm/cc.                                  ______________________________________                                    

For each run the tubular reaction system was brought up to the designated conditions. The ammonia feed was established first, then the DETA-MEA feed. After a sufficient line out period, a two hour timed run was conducted and a sample taken. The temperature was then adjusted for the next experiment. The above procedure was repeated for each of the examples.

The catalysts employed in the examples hereinafter were prepared as follows:

Catalyst A: Obtained from Norton Company, Akron, Ohio

Catalyst B: Obtained from Norton Company, Akron, Ohio.

Catalyst C: Obtained from Norton Company, Akron, Ohio.

Catalyst D: Obtained from Norton Company, Akron, Ohio.

Catalyst E: Catalyst C pellets (140 grams) were added to a solution of boric acid (5.07 grams) in methanol (94.2 grams). The methanol was removed using a Buchi rotary evaporator. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst F: Catalyst C pellets (140 grams) were added to a solution of ammonium tetrafluoroborate (2.86 grams) in water Enough solution was prepared to completely wet the pellets. The resulting slurry was allowed to stand for a period of 1 hour at room temperature. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst G: Catalyst C pellets (140.1 grams) were added to a solution of sodium tetrafluoroborate (8.58 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst H: Catalyst C pellets (140.1 grams) were added to a solution of sodium tetrafluoroborate (8.58 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst I: Catalyst C pellets (140.2 grams) were added to a solution of sodium metatungstate (1.43 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst J: Catalyst C pellets (140.2 grams) were added to a solution of sodium metatungstate (2.86 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst K: Catalyst C pellets (140.1 grams) were added to a solution of sodium metatungstate (5.71 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst L: Catalyst C pellets (140.1 grams) were added to a solution of ammonium metatungstate (3.12 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst M: Catalyst C pellets (140 grams) were added to a solution of ammonium metatungstate (6.24 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst N: Catalyst C pellets (140 1 grams) were added to a solution of ammonium metatungstate (12.48 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst O: Catalyst C pellets (140.1 rams) were added to a solution of lanthanum nitrate hexahydrate (7.59 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst P: Catalyst C pellets (143.1 grams) were added to a solution of lanthanum nitrate hexahydrate (15.18 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst Q: Catalyst C pellets (140 grams) were added to a solution of niobium pentethoxide (6.84 grams) in toluene (66 grams). Enough solution was added to completely immerse the pellets. The resulting slurry was stripped on a Buchi rotary evaporator. The catalyst was then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst R: Catalyst C pellets (140.4 grams) were added to a solution of sodium bicarbonate (3.87 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst S: Catalyst C pellets (143.5 grams) were added to a solution of vanadium triisopropoxide (7.63 grams) in toluene (66.74 grams). Enough solution was added to completely wet the pellets. The resulting slurry was stripped under reduced pressure The catalyst was then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst T: Sodium trimetaphosphate (14.0 grams) was dissolved in a sufficient amount of water (82.7 grams) to wet the TiO₂ /SiO₂ /Al₂ O₃ support (140 grams). After impregnation for a period of 1 hour at room temperature, the catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst U: Sodium trimetaphosphate (14.13 grams) was dissolved in water (56.0 grams) and isopropanol (87.0 grams). The TiO₂ /SiO₂ support (140 grams) was impregnated with the solution. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst V: Sodium trimetaphosphate (14.05 grams) was dissolved in a sufficient amount of water (85.92 grams) to wet the TiO₂ /SiO₂ support (140 grams). After impregnation for a period of 1 hour at room temperature, the catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst W: Obtained from Norton Company. Akron, Ohio.

Catalsyt X: Obtained from Norton Company, Akron, Ohio.

Catalyst Y: Obtained from Norton Company, Akron, Ohio.

Catalyst Z: Obtained from Norton Company, Akron, Ohio.

Catalsyt AA: Obtained from Norton Company, Akron, Ohio.

Catalyst BB: Obtained from Norton Company, Akron, Ohio.

Catalyst CC: Catalyst C pellets (140.5 grams) were added to a solution of zinc nitrate hexahydrate (10.45 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst DD: Catalyst C pellets (140.78 grams) were added to a solution of zinc nitrate hexahydrate (20.88 grams) in sufficient water to completely wet the pellets. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst EE: Catalyst C pellets (140.1 grams) were added to a solution of niobium pentethoxide (13.68 grams) in toluene (66.2 grams). Enough solution was added to completely immerse the pellets. The resulting slurry was allowed to stand for a period of 1 hour. The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst FF: Catalyst C pellets (140.15 grams) were added to a solution of sodium tetrafluoroborate (8.58 grams) in sufficient water to completely wet the pellets The catalyst was dried at a temperature of 100° C. for a period of 1 hour and then calcined at a temperature of 400° C. for a period of 16 hours.

Catalyst GG: Obtained from Norton Company, Akron, Ohio.

Catalyst HH: Obtained from Norton Company, Akron, Ohio.

Catalyst II: Obtained from Norton Company, Akron, Ohio.

Catalyst JJ: Obtained from Norton Company, Akron, Ohio.

                                      TABLE I                                      __________________________________________________________________________     Example No.      1   2   3   4   5   6   7   8   9                             Catalyst Type    A   A   A   A   A   A   A   A   A                             __________________________________________________________________________     Catalyst weight, gm                                                                             78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                         Pressure, psig   606 603 603 602 603 603 603 598 603                           Temperature, °C.                                                                         270 270 280 269 259 280 280 270.1                                                                              270                           Time on organics, hrs.                                                                          4.5 4.5 28.5                                                                               51.5                                                                               71.5                                                                               76.5                                                                               100.5                                                                              120 167.5                         Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           3.46                                                                               3.84                                                                               3.94                                                                               3.87                                                                               3.77                                                                               3.63                                                                               3.78                                                                               3.83                                                                               3.81                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.874                                                                              1.232                                                                              1.585                                                                              0.847                                                                              0.433                                                                              1.400                                                                              1.565                                                                              0.773                                                                              0.551                         MEA              12.473                                                                             11.945                                                                             7.517                                                                              13.370                                                                             17.877                                                                             6.436                                                                              7.199                                                                              12.823                                                                             16.111                        PIP              0.965                                                                              1.116                                                                              1.414                                                                              1.070                                                                              0.651                                                                              1.400                                                                              1.451                                                                              1.028                                                                              0.807                         DETA             39.228                                                                             39.867                                                                             35.453                                                                             41.854                                                                             47.014                                                                             35.668                                                                             35.534                                                                             41.213                                                                             44.005                        AEEA             1.227                                                                              1.108                                                                              0.479                                                                              1.371                                                                              2.399                                                                              0.486                                                                              0.502                                                                              1.388                                                                              1.922                         AEP              1.183                                                                              1.533                                                                              1.814                                                                              1.158                                                                              0.708                                                                              1.977                                                                              1.886                                                                              1.126                                                                              0.824                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.760                                                                              2.694                                                                              2.611                                                                              2.646                                                                              2.564                                                                              2.683                                                                              2.567                                                                              2.662                                                                              2.560                         1-TETA           12.867                                                                             13.297                                                                             13.364                                                                             12.613                                                                             12.062                                                                             14.170                                                                             13.658                                                                             12.943                                                                             12.257                        DAEP             0.519                                                                              0.744                                                                              0.968                                                                              0.425                                                                              0.180                                                                              1.018                                                                              0.985                                                                              0.432                                                                              0.232                         PEEDA            0.110                                                                              0.111                                                                              0.154                                                                              0.082                                                                              0.152                                                                              0.059                                                                              0.710                                                                              0.336                                                                              0.206                         DPE              0.118                                                                              0.120                                                                              0.127                                                                              0.085                                                                              0.097                                                                              0.087                                                                              0.322                                                                              0.227                                                                              0.120                         AE-TAEA          4.110                                                                              3.926                                                                              4.516                                                                              3.704                                                                              2.640                                                                              4.497                                                                              4.572                                                                              3.788                                                                              3.014                         1-TEPA           7.436                                                                              7.679                                                                              8.979                                                                              7.093                                                                              5.411                                                                              8.403                                                                              9.298                                                                              7.467                                                                              6.239                         AE-DAEP          0.140                                                                              0.117                                                                              0.182                                                                              0.100                                                                              0.097                                                                              0.000                                                                              0.808                                                                              0.390                                                                              0.275                         AE-PEEDA         0.099                                                                              0.100                                                                              0.129                                                                              0.096                                                                              0.000                                                                              0.720                                                                              0.173                                                                              0.127                                                                              0.099                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.304                                                                              0.169                                                                              0.301                                                                              0.160                                                                              0.065                                                                              0.160                                                                              1.020                                                                              0.739                                                                              0.467                         BPEA             0.639                                                                              0.578                                                                              0.844                                                                              0.573                                                                              0.045                                                                              0.211                                                                              1.060                                                                              0.835                                                                              0.435                         Others           8.068                                                                              6.841                                                                              11.264                                                                             5.414                                                                              2.775                                                                              11.735                                                                             8.190                                                                              6.222                                                                              3.695                         MEA conversion, %                                                                               66.60                                                                              68.06                                                                              79.87                                                                              63.84                                                                              52.17                                                                              82.68                                                                              80.79                                                                              66.20                                                                              56.64                         DETA conversion, %                                                                              37.56                                                                              36.64                                                                              43.59                                                                              32.72                                                                              25.25                                                                              42.94                                                                              43.64                                                                              35.44                                                                              29.62                         Acyclic(N4), wt. %                                                                              95.43                                                                              94.25                                                                              92.75                                                                              96.27                                                                              97.15                                                                              93.54                                                                              88.94                                                                              94.00                                                                              96.37                         Acyclic(N5), wt. %                                                                              90.71                                                                              92.25                                                                              90.26                                                                              92.08                                                                              97.50                                                                              92.20                                                                              81.92                                                                              84.33                                                                              87.88                         Σ (N5)/Σ(N4), weight ratio                                                          0.78                                                                               0.74                                                                               0.87                                                                               0.74                                                                               0.55                                                                               0.78                                                                               0.93                                                                               0.80                                                                               0.68                          Acyclic(N4)/cyclic(<=N4),                                                                       5.40                                                                               4.41                                                                               3.57                                                                               5.41                                                                               8.18                                                                               3.71                                                                               3.03                                                                               4.96                                                                               6.77                          weight ratio                                                                   __________________________________________________________________________     Example No.      10  11  12  13  14  15  16  17  18                            Catalyst Type    A   A   A   A   A   A   A   A   A                             __________________________________________________________________________     Catalyst weight, gm                                                                             78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                                                                              78.74                         Pressure, psig   603 604 603 604 603 603 603 604 604                           Temperature, °C.                                                                         280 259 269 260 280 270 280 270 270                           Time on organics, hrs.                                                                          172.5                                                                              191.5                                                                              196.5                                                                              214.5                                                                              219.5                                                                              238.5                                                                              243.5                                                                              262.5                                                                              266                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           3.71                                                                               3.89                                                                               3.89                                                                               3.81                                                                               3.78                                                                               3.79                                                                               3.51                                                                               3.51                                                                               3.71                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              1.445                                                                              0.461                                                                              0.791                                                                              0.658                                                                              1.456                                                                              0.910                                                                              1.122                                                                              1.072                                                                              1.017                         MEA              5.976                                                                              18.787                                                                             12.858                                                                             18.141                                                                             6.956                                                                              13.064                                                                             13.239                                                                             11.990                                                                             12.608                        PIP              1.387                                                                              0.691                                                                              1.023                                                                              0.811                                                                              1.416                                                                              1.148                                                                              1.024                                                                              1.234                                                                              1.186                         DETA             33.430                                                                             47.586                                                                             40.957                                                                             45.580                                                                             35.955                                                                             41.603                                                                             42.624                                                                             40.482                                                                             40.928                        AEEA             0.443                                                                              2.282                                                                              1.404                                                                              1.879                                                                              0.493                                                                              1.322                                                                              1.350                                                                              1.216                                                                              1.269                         AEP              1.827                                                                              0.682                                                                              1.103                                                                              0.881                                                                              1.832                                                                              1.184                                                                              1.192                                                                              1.267                                                                              1.191                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.553                                                                              2.310                                                                              2.681                                                                              2.359                                                                              2.571                                                                              2.654                                                                              2.361                                                                              2.647                                                                              2.627                         1-TETA           13.506                                                                             10.647                                                                             12.732                                                                             10.997                                                                             13.341                                                                             12.720                                                                             11.438                                                                             12.833                                                                             12.755                        DAEP             1.004                                                                              0.173                                                                              0.386                                                                              0.275                                                                              0.888                                                                              0.410                                                                              0.490                                                                              0.472                                                                              0.422                         PEEDA            0.710                                                                              0.146                                                                              0.310                                                                              0.222                                                                              0.654                                                                              0.336                                                                              0.382                                                                              0.369                                                                              0.339                         DPE              0.335                                                                              0.085                                                                              0.184                                                                              0.086                                                                              0.309                                                                              0.196                                                                              0.271                                                                              0.070                                                                              0.135                         AE-TAEA          4.645                                                                              2.372                                                                              3.629                                                                              2.706                                                                              4.368                                                                              3.735                                                                              3.951                                                                              3.951                                                                              3.751                         1-TEPA           9.538                                                                              4.500                                                                              6.990                                                                              5.378                                                                              8.945                                                                              7.412                                                                              6.576                                                                              7.610                                                                              7.246                         AE-DAEP          0.848                                                                              0.213                                                                              0.276                                                                              0.183                                                                              0.700                                                                              0.300                                                                              0.385                                                                              0.331                                                                              0.291                         AE-PEEDA         0.185                                                                              0.000                                                                              0.057                                                                              0.056                                                                              0.084                                                                              0.065                                                                              0.085                                                                              0.035                                                                              0.028                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           1.089                                                                              0.315                                                                              0.667                                                                              0.434                                                                              1.016                                                                              0.698                                                                              0.091                                                                              0.064                                                                              0.062                         BPEA             1.026                                                                              0.247                                                                              0.634                                                                              0.403                                                                              0.932                                                                              0.638                                                                              0.093                                                                              0.594                                                                              0.053                         Others           9.232                                                                              1.904                                                                              3.598                                                                              2.311                                                                              6.162                                                                              3.686                                                                              6.348                                                                              5.045                                                                              5.231                         MEA conversion, %                                                                               83.70                                                                              48.64                                                                              64.40                                                                              50.59                                                                              80.69                                                                              64.55                                                                              64.31                                                                              67.22                                                                              65.36                         DETA conversion, %                                                                              45.82                                                                              22.68                                                                              32.60                                                                              26.22                                                                              40.67                                                                              32.91                                                                              31.71                                                                              34.22                                                                              33.16                         Acyclic(N4), wt. %                                                                              88.68                                                                              96.98                                                                              94.60                                                                              95.81                                                                              89.58                                                                              94.23                                                                              92.35                                                                              94.45                                                                              94.49                         Acyclic(N5), wt. %                                                                              81.83                                                                              89.87                                                                              86.66                                                                              88.25                                                                              82.97                                                                              86.76                                                                              94.15                                                                              91.86                                                                              96.21                         Σ(N5)/Σ(N4), weight ratio                                                           0.96                                                                               0.57                                                                               0.75                                                                               0.66                                                                               0.90                                                                               0.79                                                                               0.75                                                                               0.77                                                                               0.70                          Acyclic(N4)/cyclic(<=N4),                                                                       3.05                                                                               7.29                                                                               5.13                                                                               5.86                                                                               3.12                                                                               4.70                                                                               4.11                                                                               4.54                                                                               4.70                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE II                                     __________________________________________________________________________     Example No.      19  20  21   22  23   24  25   26  27                         Catalyst Type    B   B   B    B   B    B   B    B   B                          __________________________________________________________________________     Catalyst weight, gm                                                                             84.66                                                                              84.66                                                                              84.66                                                                               84.66                                                                              84.66                                                                               84.66                                                                              84.66                                                                               84.66                                                                              84.66                      Pressure, psig   598 598 598  598 598  599 599  598 603                        Temperature, °C.                                                                         270 270 280  259 269  259 280  280 270.1                      Time on organics, hrs.                                                                          4.5 23.5                                                                               28.5 47.5                                                                               51.5 71.5                                                                               76.5 100.5                                                                              120                        Duration of run, hrs.                                                                           2   2   2    2   2    2   2    2   2                          MEA SV, gmol/hr/kgcat                                                                           2.95                                                                               2.82                                                                               2.91 2.90                                                                               2.89 2.81                                                                               2.72 2.85                                                                               2.92                       DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00                       NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97                       Crude product composition, wt. %                                               EDA              0.387                                                                              0.451                                                                              0.942                                                                               0.263                                                                              0.472                                                                               0.251                                                                              0.768                                                                               0.805                                                                              0.481                      MEA              18.211                                                                             18.550                                                                             12.561                                                                              24.117                                                                             18.908                                                                              22.270                                                                             11.181                                                                              11.851                                                                             17.815                     PIP              0.711                                                                              0.768                                                                              1.105                                                                               0.411                                                                              0.731                                                                               0.450                                                                              1.013                                                                               1.082                                                                              0.763                      DETA             45.762                                                                             47.529                                                                             39.025                                                                              52.023                                                                             46.902                                                                              51.519                                                                             38.122                                                                              38.925                                                                             46.516                     AEEA             1.902                                                                              2.077                                                                              1.192                                                                               2.582                                                                              2.111                                                                               2.804                                                                              1.247                                                                               1.088                                                                              2.005                      AEP              0.846                                                                              0.787                                                                              1.214                                                                               0.446                                                                              0.718                                                                               0.519                                                                              1.229                                                                               1.254                                                                              0.767                      HEP              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      TAEA             2.031                                                                              2.252                                                                              2.423                                                                               1.674                                                                              2.273                                                                               2.036                                                                              2.764                                                                               2.429                                                                              2.345                      1-TETA           10.921                                                                             11.106                                                                             12.012                                                                              8.125                                                                              11.140                                                                              9.812                                                                              13.613                                                                              12.691                                                                             11.657                     DAEP             0.186                                                                              0.202                                                                              0.477                                                                               0.080                                                                              0.175                                                                               0.097                                                                              0.523                                                                               0.523                                                                              0.191                      PEEDA            0.159                                                                              0.178                                                                              0.147                                                                               0.057                                                                              0.157                                                                               0.084                                                                              0.424                                                                               0.443                                                                              0.174                      DPE              0.084                                                                              0.096                                                                              0.095                                                                               0.052                                                                              0.114                                                                               0.086                                                                              0.094                                                                               0.303                                                                              0.105                      AE-TAEA          2.341                                                                              2.390                                                                              3.575                                                                               1.205                                                                              2.444                                                                               1.558                                                                              4.042                                                                               3.853                                                                              2.650                      1-TEPA           3.918                                                                              5.171                                                                              7.286                                                                               2.186                                                                              6.082                                                                               3.822                                                                              8.123                                                                               8.109                                                                              6.868                      AE-DAEP          0.366                                                                              0.189                                                                              0.131                                                                               0.129                                                                              0.081                                                                               0.000                                                                              0.417                                                                               0.508                                                                              0.093                      AE-PEEDA         0.080                                                                              0.079                                                                              0.101                                                                               0.068                                                                              0.000                                                                               0.000                                                                              0.113                                                                               0.139                                                                              0.000                      iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      AE-DPE           0.403                                                                              0.061                                                                              0.264                                                                               0.051                                                                              0.078                                                                               0.066                                                                              0.220                                                                               0.797                                                                              0.055                      BPEA             0.328                                                                              0.276                                                                              0.649                                                                               0.076                                                                              0.291                                                                               0.128                                                                              0.215                                                                               0.930                                                                              0.371                      Others           6.126                                                                              2.669                                                                              9.532                                                                               1.845                                                                              2.513                                                                               1.388                                                                              8.524                                                                               7.390                                                                              2.594                      MEA conversion, %                                                                               51.16                                                                              50.15                                                                              66.20                                                                               34.36                                                                              49.36                                                                               40.71                                                                              70.01                                                                               68.44                                                                              52.59                      DETA conversion, %                                                                              27.06                                                                              24.09                                                                              37.59                                                                               15.85                                                                              25.35                                                                               18.49                                                                              39.22                                                                               38.40                                                                              26.43                      Acyclic(N4), wt. %                                                                              96.80                                                                              96.56                                                                              95.26                                                                               98.11                                                                              96.78                                                                               97.79                                                                              94.03                                                                               92.26                                                                              96.75                      Acyclic(N5), wt. %                                                                              84.17                                                                              92.59                                                                              90.47                                                                               91.27                                                                              94.99                                                                               96.53                                                                              92.65                                                                               83.44                                                                              94.83                      Σ (N5)/Σ(N4), weight ratio                                                          0.56                                                                               0.59                                                                               0.79 0.37                                                                               0.65 0.46                                                                               0.75 0.87                                                                               0.69                       Acyclic(N4)/cyclic(<=N4),                                                                       6.52                                                                               6.58                                                                               4.75 9.37                                                                               7.08 9.58                                                                               4.99 4.20                                                                               7.00                       weight ratio                                                                   __________________________________________________________________________     Example No.      28  29  30  31  32  33  34  35  36  37                        Catalyst Type    B   B   B   B   B   B   B   B   B   B                         __________________________________________________________________________     Catalyst weight, gm                                                                             84.66                                                                              84.66                                                                              84.66                                                                              84.66                                                                              84.66                                                                              84.66                                                                              84.66                                                                              84.66                                                                              84.66                                                                              84.66                     Pressure, psig   598 598 598 598 598 599 599 604 604 604                       Temperature, °C.                                                                         270 280 259 269 260 280 270 280 270 270                       Time on organics, hrs.                                                                          167.5                                                                              172.5                                                                              191.5                                                                              196.5                                                                              214.5                                                                              219.5                                                                              238.5                                                                              243.5                                                                              262.5                                                                              266                       Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           2.92                                                                               2.51                                                                               2.94                                                                               2.91                                                                               3.37                                                                               2.82                                                                               2.90                                                                               2.83                                                                               2.69                                                                               2.83                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              0.768                                                                              0.935                                                                              0.259                                                                              0.554                                                                              0.303                                                                              0.984                                                                              0.731                                                                              1.166                                                                              0.772                                                                              0.727                     MEA              11.617                                                                             9.895                                                                              22.504                                                                             16.654                                                                             25.518                                                                             10.278                                                                             15.594                                                                             9.688                                                                              14.486                                                                             15.223                    PIP              1.012                                                                              1.112                                                                              0.501                                                                              0.801                                                                              0.351                                                                              1.163                                                                              0.969                                                                              1.258                                                                              0.984                                                                              0.967                     DETA             38.660                                                                             37.291                                                                             50.906                                                                             44.882                                                                             53.431                                                                             38.532                                                                             43.211                                                                             37.652                                                                             42.240                                                                             43.621                    AEEA             1.321                                                                              0.909                                                                              2.608                                                                              1.955                                                                              2.502                                                                              0.852                                                                              1.707                                                                              0.755                                                                              1.601                                                                              1.652                     AEP              1.097                                                                              1.308                                                                              0.480                                                                              0.827                                                                              0.406                                                                              1.361                                                                              1.004                                                                              1.440                                                                              1.010                                                                              0.980                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             2.638                                                                              2.623                                                                              2.028                                                                              2.607                                                                              1.424                                                                              2.641                                                                              2.659                                                                              2.671                                                                              2.744                                                                              2.666                     1-TETA           12.643                                                                             12.534                                                                             9.067                                                                              11.734                                                                             6.423                                                                              12.393                                                                             11.936                                                                             12.701                                                                             12.439                                                                             12.081                    DAEP             0.461                                                                              0.560                                                                              0.119                                                                              0.241                                                                              0.079                                                                              0.538                                                                              0.298                                                                              0.622                                                                              0.320                                                                              0.282                     PEEDA            0.353                                                                              0.455                                                                              0.081                                                                              0.211                                                                              0.068                                                                              0.431                                                                              0.263                                                                              0.498                                                                              0.276                                                                              0.248                     DPE              0.353                                                                              0.332                                                                              0.103                                                                              0.133                                                                              0.127                                                                              0.308                                                                              0.161                                                                              0.109                                                                              0.118                                                                              0.100                     AE-TAEA          3.917                                                                              4.248                                                                              1.719                                                                              2.992                                                                              1.105                                                                              4.215                                                                              3.423                                                                              4.647                                                                              3.605                                                                              3.411                     1-TEPA           8.051                                                                              8.471                                                                              3.147                                                                              5.870                                                                              1.995                                                                              8.144                                                                              6.762                                                                              8.696                                                                              6.609                                                                              6.249                     AE-DAEP          0.479                                                                              0.536                                                                              0.073                                                                              0.161                                                                              0.074                                                                              0.499                                                                              0.236                                                                              0.581                                                                              0.204                                                                              0.181                     AE-PEEDA         0.163                                                                              0.150                                                                              0.064                                                                              0.000                                                                              0.053                                                                              0.132                                                                              0.054                                                                              0.123                                                                              0.034                                                                              0.030                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.793                                                                              0.918                                                                              0.151                                                                              0.456                                                                              0.092                                                                              0.892                                                                              0.536                                                                              0.306                                                                              0.061                                                                              0.063                     BPEA             0.949                                                                              1.033                                                                              0.115                                                                              0.459                                                                              0.108                                                                              0.885                                                                              0.576                                                                              0.724                                                                              0.059                                                                              0.402                     Others           7.450                                                                              7.630                                                                              1.713                                                                              2.553                                                                              2.042                                                                              6.020                                                                              3.491                                                                              7.953                                                                              4.671                                                                              3.839                     MEA conversion, %                                                                               68.95                                                                              73.17                                                                              39.26                                                                              54.71                                                                              30.82                                                                              71.85                                                                              58.06                                                                              73.87                                                                              60.45                                                                              58.58                     DETA conversion, %                                                                              38.60                                                                              39.91                                                                              18.34                                                                              27.46                                                                              13.91                                                                              37.28                                                                              30.93                                                                              39.64                                                                              31.46                                                                              29.46                     Acyclic(N4), wt. %                                                                              92.90                                                                              91.84                                                                              97.34                                                                              96.08                                                                              96.64                                                                              92.17                                                                              95.29                                                                              92.60                                                                              95.51                                                                              95.90                     Acyclic(N5), wt. %                                                                              83.45                                                                              82.83                                                                              92.34                                                                              89.17                                                                              90.46                                                                              83.69                                                                              87.90                                                                              88.50                                                                              96.63                                                                              93.47                     Σ(N5)/Σ(N4), weight ratio                                                           0.88                                                                               0.93                                                                               0.46                                                                               0.67                                                                               0.42                                                                               0.91                                                                               0.76                                                                               0.91                                                                               0.67                                                                               0.67                      Acyclic(N4)/cyclic(<=N4),                                                                       4.66                                                                               4.02                                                                               8.64                                                                               6.48                                                                               7.62                                                                               3.95                                                                               5.42                                                                               3.91                                                                               5.61                                                                               5.72                      weight ratio                                                                   __________________________________________________________________________

                                      TABLE III                                    __________________________________________________________________________     Example No.      38  39  40  41  42  43  44  45  46                            Catalyst Type    C   C   C   C   C   C   C   C   C                             __________________________________________________________________________     Catalyst weight, gm                                                                             75  75  75  75  75  75  75  75  75                            Pressure, psig   607.5                                                                              600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         267.9                                                                              267.8                                                                              277.8                                                                              259.9                                                                              270.1                                                                              259.9                                                                              280.1                                                                              269.6                                                                              269                           Time on organics, hrs.                                                                          5   7.5 26  31.5                                                                               50  55.5                                                                               74  78  80                            Duration of run, hrs.                                                                           1   1   2   2   2   2   2   2   1.5                           MEA SV, gmol/hr/kgcat                                                                           8.48                                                                               8.57                                                                               4.17                                                                               3.96                                                                               3.90                                                                               4.22                                                                               4.15                                                                               4.01                                                                               3.97                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.673                                                                              0.822                                                                              1.742                                                                              0.612                                                                              1.367                                                                              0.688                                                                              2.430                                                                              1.370                                                                              1.341                         MEA              33.641                                                                             24.246                                                                             13.234                                                                             26.804                                                                             16.396                                                                             24.443                                                                             8.046                                                                              15.672                                                                             15.462                        PIP              0.585                                                                              1.113                                                                              0.000                                                                              0.823                                                                              1.584                                                                              0.886                                                                              1.994                                                                              1.506                                                                              1.484                         DETA             51.838                                                                             49.325                                                                             40.936                                                                             52.117                                                                             49.168                                                                             51.098                                                                             40.046                                                                             47.408                                                                             47.941                        AEEA             2.205                                                                              0.926                                                                              0.312                                                                              1.512                                                                              0.754                                                                              1.506                                                                              0.202                                                                              0.925                                                                              0.850                         AEP              0.502                                                                              0.953                                                                              1.969                                                                              0.613                                                                              1.431                                                                              0.666                                                                              2.287                                                                              1.330                                                                              1.326                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             0.488                                                                              2.104                                                                              2.220                                                                              1.660                                                                              2.270                                                                              1.751                                                                              2.342                                                                              2.219                                                                              2.195                         1-TETA           4.586                                                                              9.252                                                                              11.293                                                                             7.569                                                                              10.817                                                                             7.792                                                                              12.031                                                                             10.555                                                                             10.356                        DAEP             0.000                                                                              0.167                                                                              0.922                                                                              0.114                                                                              0.307                                                                              0.112                                                                              1.101                                                                              0.290                                                                              0.271                         PEEDA            0.000                                                                              0.113                                                                              0.678                                                                              0.000                                                                              0.217                                                                              0.075                                                                              0.791                                                                              0.209                                                                              0.196                         DPE              0.000                                                                              0.000                                                                              0.205                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.096                                                                              0.000                                                                              0.000                         AE-TAEA          0.234                                                                              1.259                                                                              3.575                                                                              0.885                                                                              2.431                                                                              1.011                                                                              3.561                                                                              2.057                                                                              2.091                         1-TEPA           0.541                                                                              2.471                                                                              6.977                                                                              1.667                                                                              5.274                                                                              1.895                                                                              7.683                                                                              4.176                                                                              3.991                         AE-DAEP          0.000                                                                              0.000                                                                              0.676                                                                              0.000                                                                              0.134                                                                              0.000                                                                              0.783                                                                              0.149                                                                              0.124                         AE-PEEDA         0.000                                                                              0.000                                                                              0.710                                                                              0.000                                                                              0.089                                                                              0.000                                                                              0.718                                                                              0.000                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.000                                                                              0.000                                                                              0.882                                                                              0.000                                                                              0.270                                                                              0.091                                                                              1.072                                                                              0.423                                                                              0.395                         BPEA             0.000                                                                              0.000                                                                              0.729                                                                              0.000                                                                              0.340                                                                              0.077                                                                              0.874                                                                              0.385                                                                              0.362                         Others           0.455                                                                              0.399                                                                              3.890                                                                              0.125                                                                              1.112                                                                              0.488                                                                              5.301                                                                              1.685                                                                              1.506                         MEA conversion, %                                                                               6.59                                                                               32.47                                                                              63.69                                                                              25.82                                                                              54.29                                                                              31.29                                                                              78.37                                                                              56.01                                                                              56.32                         DETA conversion, %                                                                              14.45                                                                              18.36                                                                              33.25                                                                              14.28                                                                              23.51                                                                              14.64                                                                              36.03                                                                              20.92                                                                              19.52                         Acyclic(N4), wt. %                                                                              100.00                                                                             97.59                                                                              88.22                                                                              98.78                                                                              96.15                                                                              98.08                                                                              87.85                                                                              96.23                                                                              96.41                         Acyclic(N5), wt. %                                                                              100.00                                                                             100.00                                                                             77.88                                                                              100.00                                                                             90.24                                                                              94.53                                                                              76.53                                                                              86.69                                                                              87.22                         Σ(N5)/Σ (N4), weight ratio                                                          0.15                                                                               0.32                                                                               0.88                                                                               0.27                                                                               0.63                                                                               0.32                                                                               0.90                                                                               0.54                                                                               0.53                          Acyclic(N4)/cyclic(<=N4),                                                                       4.67                                                                               4.84                                                                               3.58                                                                               5.96                                                                               3.70                                                                               5.49                                                                               2.29                                                                               3.83                                                                               3.83                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE IV                                     __________________________________________________________________________     Example No.      47  48  49   50  51   52  53   54  55                         Catalyst Type    D   D   D    D   D    D   D    D   D                          __________________________________________________________________________     Catalyst weight, gm                                                                             68.38                                                                              68.38                                                                              68.38                                                                               68.38                                                                              68.38                                                                               68.38                                                                              68.38                                                                               68.38                                                                              68.38                      Pressure, psig   602 602 602  602 602  603 603  602 602                        Temperature, °C.                                                                         270 270 280  259 269  259 280  280 270.1                      Time on organics, hrs.                                                                          4.5 23.5                                                                               28.5 47.5                                                                               51.5 71.5                                                                               76.5 100.5                                                                              120                        Duration of run, hrs.                                                                           2   2   2    2   2    2   2    2   2                          MEA SV, gmol/hr/kgcat                                                                           3.96                                                                               3.87                                                                               4.09 3.96                                                                               3.90 3.87                                                                               3.92 3.90                                                                               4.03                       DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00                       NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97                       Crude product composition, wt. %                                               EDA              0.223                                                                              0.361                                                                              0.675                                                                               0.212                                                                              0.396                                                                               0.180                                                                              0.730                                                                               0.795                                                                              0.461                      MEA              24.445                                                                             22.069                                                                             16.449                                                                              26.799                                                                             21.362                                                                              24.727                                                                             13.740                                                                              14.037                                                                             20.260                     PIP              0.470                                                                              0.526                                                                              0.892                                                                               0.297                                                                              0.553                                                                               0.298                                                                              0.888                                                                               0.897                                                                              0.585                      DETA             53.878                                                                             51.806                                                                             46.950                                                                              56.278                                                                             50.889                                                                              55.710                                                                             44.046                                                                              42.839                                                                             49.907                     AEEA             2.281                                                                              2.479                                                                              1.818                                                                               2.578                                                                              2.565                                                                               2.914                                                                              1.871                                                                               1.449                                                                              2.318                      AEP              0.515                                                                              0.624                                                                              1.064                                                                               0.387                                                                              0.663                                                                               0.447                                                                              1.193                                                                               1.137                                                                              0.672                      HEP              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      TAEA             1.420                                                                              1.640                                                                              2.118                                                                               1.210                                                                              1.747                                                                               1.411                                                                              2.465                                                                               2.237                                                                              1.931                      1-TETA           7.238                                                                              7.768                                                                              10.879                                                                              5.638                                                                              8.217                                                                               6.704                                                                              12.235                                                                              11.091                                                                             9.032                      DAEP             0.092                                                                              0.160                                                                              0.324                                                                               0.058                                                                              0.188                                                                               0.079                                                                              0.480                                                                               0.476                                                                              0.204                      PEEDA            0.097                                                                              0.137                                                                              0.289                                                                               0.053                                                                              0.154                                                                               0.073                                                                              0.398                                                                               0.393                                                                              0.166                      DPE              0.075                                                                              0.095                                                                              0.046                                                                               0.052                                                                              0.063                                                                               0.100                                                                              0.355                                                                               0.333                                                                              0.191                      AE-TAEA          1.219                                                                              1.522                                                                              2.583                                                                               0.752                                                                              1.679                                                                               0.945                                                                              3.598                                                                               3.115                                                                              2.003                      1-TEPA           2.039                                                                              2.628                                                                              5.427                                                                               1.366                                                                              3.512                                                                               1.934                                                                              6.530                                                                               6.472                                                                              4.096                      AE-DAEP          0.173                                                                              0.187                                                                              0.318                                                                               0.000                                                                              0.179                                                                               0.087                                                                              0.390                                                                               0.491                                                                              0.208                      AE-PEEDA         0.066                                                                              0.063                                                                              0.068                                                                               0.000                                                                              0.071                                                                               0.080                                                                              0.096                                                                               0.129                                                                              0.079                      iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      AE-DPE           0.141                                                                              0.121                                                                              0.160                                                                               0.073                                                                              0.175                                                                               0.115                                                                              0.175                                                                               0.301                                                                              0.139                      BPEA             0.101                                                                              0.141                                                                              0.381                                                                               0.047                                                                              0.197                                                                               0.060                                                                              0.186                                                                               0.732                                                                              0.292                      Others           2.821                                                                              3.594                                                                              4.790                                                                               1.260                                                                              3.582                                                                               1.974                                                                              6.576                                                                               7.895                                                                              3.856                      MEA conversion, %                                                                               34.76                                                                              40.66                                                                              56.27                                                                               27.73                                                                              42.89                                                                               34.28                                                                              64.11                                                                               62.93                                                                              46.18                      DETA conversion, %                                                                              14.55                                                                              17.21                                                                              25.83                                                                               9.80                                                                               19.14                                                                               12.00                                                                              31.61                                                                               32.77                                                                              21.21                      Acyclic(N4), wt. %                                                                              97.05                                                                              96.00                                                                              95.18                                                                               97.67                                                                              96.10                                                                               96.98                                                                              92.27                                                                               91.72                                                                              95.13                      Acyclic(N5), wt. %                                                                              87.14                                                                              89.01                                                                              89.63                                                                               94.66                                                                              89.31                                                                               89.37                                                                              92.28                                                                               85.30                                                                              89.48                      Σ(N5)/Σ(N4), weight ratio                                                           0.42                                                                               0.48                                                                               0.65 0.32                                                                               0.56 0.38                                                                               0.69 0.77                                                                               0.59                       Acyclic(N4)/cyclic(<=N4),                                                                       7.31                                                                               6.11                                                                               4.97 8.08                                                                               6.15 8.14                                                                               4.44 4.12                                                                               6.03                       weight ratio                                                                   __________________________________________________________________________     Example No.      56  57  58  59  60  61  62  63  64  65                        Catalyst Type    D   D   D   D   D   D   D   D   D   D                         __________________________________________________________________________     Catalyst weight, gm                                                                             68.38                                                                              68.38                                                                              68.38                                                                              68.38                                                                              68.38                                                                              68.38                                                                              68.38                                                                              68.38                                                                              68.38                                                                              68.38                     Pressure, psig   602 602 603 602 603 603 602 603 603 603                       Temperature, °C.                                                                         270 280 259 269 260 280 270 280 270 270                       Time on organics, hrs.                                                                          167.5                                                                              172.5                                                                              191.5                                                                              196.5                                                                              214.5                                                                              219.5                                                                              238.5                                                                              243.5                                                                              262.5                                                                              266                       Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           3.92                                                                               3.98                                                                               4.05                                                                               4.06                                                                               3.59                                                                               4.00                                                                               3.95                                                                               4.40                                                                               3.76                                                                               3.89                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              0.516                                                                              0.878                                                                              0.251                                                                              0.489                                                                              0.337                                                                              0.945                                                                              0.600                                                                              1.593                                                                              0.706                                                                              0.676                     MEA              18.745                                                                             12.739                                                                             24.769                                                                             19.980                                                                             21.647                                                                             14.371                                                                             19.473                                                                             6.716                                                                              18.311                                                                             19.235                    PIP              0.611                                                                              0.931                                                                              0.340                                                                              0.589                                                                              0.483                                                                              0.985                                                                              0.679                                                                              1.480                                                                              0.743                                                                              0.731                     DETA             47.493                                                                             41.921                                                                             53.539                                                                             49.348                                                                             49.438                                                                             44.879                                                                             48.790                                                                             36.170                                                                             47.421                                                                             48.217                    AEEA             2.331                                                                              1.424                                                                              2.555                                                                              2.352                                                                              2.505                                                                              1.539                                                                              2.260                                                                              0.475                                                                              2.170                                                                              2.155                     AEP              0.691                                                                              1.141                                                                              0.402                                                                              0.686                                                                              0.479                                                                              1.175                                                                              0.770                                                                              1.905                                                                              0.803                                                                              0.752                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             2.040                                                                              2.361                                                                              1.480                                                                              1.962                                                                              2.037                                                                              2.311                                                                              2.070                                                                              2.556                                                                              2.174                                                                              1.990                     1-TETA           9.416                                                                              11.410                                                                             6.735                                                                              8.956                                                                              8.928                                                                              10.980                                                                             9.466                                                                              13.448                                                                             10.036                                                                             9.225                     DAEP             0.223                                                                              0.454                                                                              0.082                                                                              0.179                                                                              0.113                                                                              0.411                                                                              0.216                                                                              0.992                                                                              0.260                                                                              0.214                     PEEDA            0.181                                                                              0.371                                                                              0.072                                                                              0.153                                                                              0.087                                                                              0.337                                                                              0.181                                                                              0.685                                                                              0.205                                                                              0.176                     DPE              0.211                                                                              0.323                                                                              0.103                                                                              0.188                                                                              0.090                                                                              0.336                                                                              0.229                                                                              0.084                                                                              0.151                                                                              0.130                     AE-TAEA          2.229                                                                              3.445                                                                              1.148                                                                              1.988                                                                              1.704                                                                              3.208                                                                              2.190                                                                              4.698                                                                              2.609                                                                              2.255                     1-TEPA           4.517                                                                              6.679                                                                              2.110                                                                              3.632                                                                              3.226                                                                              6.048                                                                              4.274                                                                              8.949                                                                              4.512                                                                              4.130                     AE-DAEP          0.250                                                                              0.419                                                                              0.072                                                                              0.068                                                                              0.065                                                                              0.302                                                                              0.149                                                                              0.729                                                                              0.156                                                                              0.129                     AE-PEEDA         0.091                                                                              0.113                                                                              0.055                                                                              0.000                                                                              0.051                                                                              0.055                                                                              0.000                                                                              0.083                                                                              0.027                                                                              0.026                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.100                                                                              0.642                                                                              0.059                                                                              0.074                                                                              0.169                                                                              0.596                                                                              0.296                                                                              0.104                                                                              0.073                                                                              0.070                     BPEA             0.316                                                                              0.649                                                                              0.081                                                                              0.221                                                                              0.152                                                                              0.558                                                                              0.257                                                                              0.781                                                                              0.053                                                                              0.056                     Others           4.550                                                                              5.879                                                                              1.898                                                                              3.066                                                                              1.779                                                                              4.582                                                                              3.140                                                                              7.552                                                                              4.192                                                                              3.803                     MEA conversion, %                                                                               49.40                                                                              65.33                                                                              32.69                                                                              45.43                                                                              40.15                                                                              61.44                                                                              47.63                                                                              81.50                                                                              50.64                                                                              47.61                     DETA conversion, %                                                                              23.81                                                                              32.19                                                                              13.53                                                                              19.90                                                                              18.77                                                                              28.43                                                                              22.01                                                                              40.80                                                                              24.03                                                                              21.95                     Acyclic(N4), wt. %                                                                              94.90                                                                              92.30                                                                              96.97                                                                              95.46                                                                              97.43                                                                              92.46                                                                              94.85                                                                              90.08                                                                              95.20                                                                              95.57                     Acyclic(N5), wt. %                                                                              89.91                                                                              84.74                                                                              92.45                                                                              93.93                                                                              91.87                                                                              85.96                                                                              90.20                                                                              88.94                                                                              95.85                                                                              95.78                     Σ(N5)/Σ(N4), weight ratio                                                           0.62                                                                               0.80                                                                               0.42                                                                               0.52                                                                               0.48                                                                               0.75                                                                               0.59                                                                               0.86                                                                               0.58                                                                               0.57                      Acyclic(N4)/cyclic(<=N4),                                                                       5.98                                                                               4.28                                                                               8.23                                                                               6.09                                                                               8.76                                                                               4.10                                                                               5.56                                                                               3.11                                                                               5.65                                                                               5.60                      weight ratio                                                                   __________________________________________________________________________

                                      TABLE V                                      __________________________________________________________________________     Example No.      66  67  68  69  70  71  72  73  74                            Catalyst Type    E   E   E   E   E   E   E   E   E                             __________________________________________________________________________     Catalyst weight, gm                                                                             73.5                                                                               73.5                                                                               73.5                                                                               73.5                                                                               73.5                                                                               73.5                                                                               73.5                                                                               73.5                                                                               73.5                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         271.8                                                                              270 280.2                                                                              260.9                                                                              270.6                                                                              261.2                                                                              281.5                                                                              270 270                           Time on organics, hrs.                                                                          5   8.5 25  30  34  49  55  76  78                            Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           4.58                                                                               4.68                                                                               4.69                                                                               4.82                                                                               4.64                                                                               4.33                                                                               4.30                                                                               4.25                                                                               4.63                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              1.589                                                                              2.650                                                                              2.164                                                                              0.505                                                                              0.958                                                                              0.544                                                                              2.028                                                                              0.834                                                                              1.373                         MEA              12.185                                                                             10.223                                                                             10.619                                                                             22.868                                                                             16.851                                                                             21.648                                                                             7.865                                                                              11.872                                                                             15.153                        PIP              1.766                                                                              1.979                                                                              2.007                                                                              0.826                                                                              1.277                                                                              0.872                                                                              2.020                                                                              1.302                                                                              1.673                         DETA             50.183                                                                             46.166                                                                             46.617                                                                             54.246                                                                             49.991                                                                             54.106                                                                             39.033                                                                             47.518                                                                             46.832                        AEEA             0.119                                                                              0.000                                                                              0.000                                                                              0.956                                                                              0.608                                                                              1.198                                                                              0.102                                                                              0.526                                                                              0.540                         AEP              2.179                                                                              2.940                                                                              2.249                                                                              0.787                                                                              1.410                                                                              0.884                                                                              2.331                                                                              1.655                                                                              1.577                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.287                                                                              2.018                                                                              2.378                                                                              1.970                                                                              2.298                                                                              2.027                                                                              2.600                                                                              2.786                                                                              2.092                         1-TETA           11.888                                                                             11.231                                                                             12.228                                                                             9.216                                                                              11.514                                                                             9.474                                                                              13.657                                                                             14.189                                                                             11.667                        DAEP             0.650                                                                              1.480                                                                              0.908                                                                              0.125                                                                              0.263                                                                              0.142                                                                              1.136                                                                              0.460                                                                              0.271                         PEEDA            0.395                                                                              0.990                                                                              0.562                                                                              0.087                                                                              0.186                                                                              0.092                                                                              0.793                                                                              0.320                                                                              0.185                         DPE              0.000                                                                              0.079                                                                              0.082                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.063                                                                              0.000                                                                              0.000                         AE-TAEA          2.483                                                                              2.485                                                                              2.951                                                                              1.171                                                                              2.213                                                                              1.284                                                                              3.723                                                                              3.229                                                                              2.178                         1-TEPA           5.189                                                                              5.996                                                                              6.225                                                                              2.266                                                                              4.333                                                                              2.454                                                                              8.413                                                                              6.752                                                                              4.536                         AE-DAEP          0.456                                                                              1.010                                                                              0.453                                                                              0.000                                                                              0.214                                                                              0.000                                                                              0.650                                                                              0.175                                                                              0.435                         AE-PEEDA         0.128                                                                              0.369                                                                              0.129                                                                              0.000                                                                              0.181                                                                              0.000                                                                              0.200                                                                              0.000                                                                              0.419                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.131                                                                              0.143                                                                              0.206                                                                              0.000                                                                              0.132                                                                              0.000                                                                              0.735                                                                              0.194                                                                              0.412                         BPEA             0.097                                                                              0.158                                                                              0.137                                                                              0.000                                                                              0.160                                                                              0.000                                                                              0.654                                                                              0.211                                                                              0.541                         Others           0.955                                                                              2.634                                                                              1.884                                                                              0.416                                                                              0.810                                                                              0.314                                                                              3.399                                                                              0.747                                                                              2.735                         MEA conversion, %                                                                               67.00                                                                              72.55                                                                              71.14                                                                              37.96                                                                              54.14                                                                              41.18                                                                              78.38                                                                              67.95                                                                              58.74                         DETA conversion, %                                                                              19.21                                                                              26.33                                                                              24.71                                                                              12.54                                                                              19.15                                                                              12.63                                                                              36.23                                                                              23.77                                                                              24.21                         Acyclic(N4), wt. %                                                                              93.14                                                                              83.87                                                                              90.40                                                                              98.14                                                                              96.85                                                                              98.00                                                                              89.08                                                                              95.60                                                                              96.79                         Acyclic(N5), wt. %                                                                              90.43                                                                              83.47                                                                              90.84                                                                              100.00                                                                             90.50                                                                              100.00                                                                             84.43                                                                              94.51                                                                              78.79                         Σ (N5)/Σ(N4), weight ratio                                                          0.56                                                                               0.64                                                                               0.63                                                                               0.30                                                                               0.51                                                                               0.32                                                                               0.79                                                                               0.59                                                                               0.60                          Acyclic(N4)/cyclic(<=N4),                                                                       2.84                                                                               1.77                                                                               2.51                                                                               6.13                                                                               4.40                                                                               5.78                                                                               2.57                                                                               4.54                                                                               3.71                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE VI                                     __________________________________________________________________________     Example No.      75  76  77  78  79  80  81  82  83                            Catalyst Type    F   F   F   F   F   F   F   F   F                             __________________________________________________________________________     Catalyst weight, gm                                                                             76.8                                                                               76.8                                                                               76.8                                                                               76.8                                                                               76.8                                                                               76.8                                                                               76.8                                                                               76.8                                                                               76.8                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         271.8                                                                              270 280.2                                                                              260.9                                                                              270.6                                                                              261.2                                                                              281.5                                                                              270 270                           Time on organics, hrs.                                                                          5   8.5 25  30  34  49  55  76  78                            Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           4.12                                                                               4.24                                                                               4.01                                                                               4.36                                                                               4.32                                                                               4.20                                                                               4.12                                                                               4.07                                                                               4.24                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.668                                                                              1.225                                                                              4.618                                                                              0.557                                                                              0.985                                                                              0.575                                                                              1.947                                                                              0.795                                                                              1.103                         MEA              20.080                                                                             14.935                                                                             10.851                                                                             24.320                                                                             17.690                                                                             22.023                                                                             6.480                                                                              10.724                                                                             12.429                        PIP              0.842                                                                              1.211                                                                              3.467                                                                              0.742                                                                              1.218                                                                              0.827                                                                              1.830                                                                              1.251                                                                              1.391                         DETA             54.453                                                                             48.042                                                                             42.353                                                                             55.896                                                                             51.741                                                                             52.738                                                                             44.334                                                                             45.995                                                                             43.281                        AEEA             0.451                                                                              0.313                                                                              0.139                                                                              1.169                                                                              0.760                                                                              1.449                                                                              0.113                                                                              0.560                                                                              0.651                         AEP              0.974                                                                              1.563                                                                              4.537                                                                              0.688                                                                              1.325                                                                              0.757                                                                              2.402                                                                              1.604                                                                              1.454                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.048                                                                              2.361                                                                              1.079                                                                              1.584                                                                              2.048                                                                              1.917                                                                              2.309                                                                              2.717                                                                              2.272                         1-TETA           10.507                                                                             12.537                                                                             9.182                                                                              8.077                                                                              10.742                                                                             9.822                                                                              13.034                                                                             15.283                                                                             13.463                        DAEP             0.193                                                                              0.511                                                                              1.628                                                                              0.101                                                                              0.256                                                                              0.153                                                                              0.989                                                                              0.531                                                                              0.365                         PEEDA            0.122                                                                              0.327                                                                              1.082                                                                              0.000                                                                              0.173                                                                              0.087                                                                              0.592                                                                              0.336                                                                              0.226                         DPE              0.000                                                                              0.000                                                                              0.152                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.071                                                                              0.000                                                                              0.000                         AE-TAEA          1.448                                                                              2.895                                                                              1.930                                                                              0.722                                                                              1.679                                                                              1.331                                                                              3.231                                                                              3.219                                                                              2.996                         1-TEPA           2.807                                                                              6.158                                                                              3.803                                                                              1.591                                                                              3.499                                                                              2.971                                                                              7.631                                                                              7.644                                                                              6.601                         AE-DAEP          0.000                                                                              0.383                                                                              1.217                                                                              0.000                                                                              0.082                                                                              0.000                                                                              0.605                                                                              0.208                                                                              0.516                         AE-PEEDA         0.000                                                                              0.091                                                                              0.346                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.174                                                                              0.000                                                                              0.418                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.000                                                                              0.211                                                                              0.255                                                                              0.000                                                                              0.095                                                                              0.000                                                                              0.622                                                                              0.212                                                                              0.696                         BPEA             0.000                                                                              0.119                                                                              0.152                                                                              0.000                                                                              0.089                                                                              0.000                                                                              0.573                                                                              0.168                                                                              0.136                         Others           0.356                                                                              1.079                                                                              3.709                                                                              0.353                                                                              0.618                                                                              0.261                                                                              2.961                                                                              0.934                                                                              4.252                         MEA conversion, %                                                                               45.60                                                                              59.89                                                                              70.22                                                                              33.93                                                                              51.41                                                                              40.05                                                                              82.26                                                                              70.97                                                                              66.33                         DETA conversion, %                                                                              12.33                                                                              23.33                                                                              30.92                                                                              9.75                                                                               15.54                                                                              14.68                                                                              27.88                                                                              26.01                                                                              30.31                         Acyclic(N4), wt. %                                                                              97.56                                                                              94.68                                                                              78.19                                                                              98.96                                                                              96.75                                                                              97.99                                                                              90.27                                                                              95.40                                                                              96.38                         Acyclic(N5), wt. %                                                                              100.00                                                                             91.84                                                                              74.42                                                                              100.00                                                                             95.12                                                                              100.00                                                                             84.62                                                                              94.86                                                                              84.46                         Σ(N5)/Σ (N4), weight ratio                                                          0.33                                                                               0.63                                                                               0.59                                                                               0.24                                                                               0.41                                                                               0.36                                                                               0.76                                                                               0.61                                                                               0.70                          Acyclic(N4)/cyclic(<=N4),                                                                       5.89                                                                               4.12                                                                               0.94                                                                               6.31                                                                               4.30                                                                               6.43                                                                               2.61                                                                               4.84                                                                               4.58                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE VII                                    __________________________________________________________________________     Example No.      84  85  86  87  88  89  90  91                                Catalyst Type    G   G   G   G   G   G   G   G                                 __________________________________________________________________________     Catalyst weight, gm                                                                             76.9                                                                               76.9                                                                               76.9                                                                               76.9                                                                               76.9                                                                               76.9                                                                               76.9                                                                               76.9                              Pressure, psig   600 600 600 600 600 600 600 600                               Temperature, °C.                                                                         274.4                                                                              274.4                                                                              280.9                                                                              259.8                                                                              270.6                                                                              259.9                                                                              281.6                                                                              270.4                             Time on organics, hrs.                                                                          22  26  45.5                                                                               50.5                                                                               69  74.5                                                                               95  119                               Duration of run, hrs.                                                                           2   2   2   2   2   2   2   1                                 MEA SV, gmol/hr/kgcat                                                                           3.43                                                                               3.31                                                                               2.85                                                                               3.38                                                                               3.41                                                                               3.28                                                                               3.10                                                                               3.37                              DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                              NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                              Crude product composition, wt. %                                               EDA              1.637                                                                              1.752                                                                              6.215                                                                              1.030                                                                              1.705                                                                              0.900                                                                              2.931                                                                              2.193                             MEA              11.346                                                                             11.171                                                                             3.117                                                                              18.167                                                                             8.987                                                                              15.534                                                                             1.812                                                                              8.349                             PIP              0.000                                                                              1.648                                                                              4.753                                                                              1.076                                                                              1.772                                                                              1.117                                                                              2.704                                                                              1.830                             DETA             46.167                                                                             45.574                                                                             31.042                                                                             48.855                                                                             44.146                                                                             47.263                                                                             56.512                                                                             40.724                            AEEA             0.707                                                                              0.779                                                                              0.145                                                                              2.493                                                                              0.622                                                                              2.337                                                                              0.000                                                                              0.571                             AEP              1.861                                                                              1.810                                                                              7.515                                                                              1.125                                                                              2.031                                                                              1.205                                                                              4.394                                                                              2.315                             HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                             TAEA             2.681                                                                              2.785                                                                              1.354                                                                              2.334                                                                              2.745                                                                              2.609                                                                              1.349                                                                              2.559                             1-TETA           14.827                                                                             14.769                                                                             9.178                                                                              13.329                                                                             15.519                                                                             14.514                                                                             14.115                                                                             14.634                            DAEP             0.707                                                                              0.684                                                                              3.204                                                                              0.266                                                                              0.862                                                                              0.288                                                                              1.482                                                                              1.224                             PEEDA            0.445                                                                              0.480                                                                              2.063                                                                              0.161                                                                              0.535                                                                              0.170                                                                              0.741                                                                              0.805                             DPE              0.104                                                                              0.070                                                                              0.140                                                                              0.000                                                                              0.097                                                                              0.000                                                                              0.000                                                                              0.048                             AE-TAEA          2.754                                                                              2.700                                                                              1.519                                                                              1.536                                                                              2.882                                                                              1.909                                                                              0.548                                                                              2.624                             1-TEPA           6.335                                                                              6.366                                                                              3.932                                                                              3.904                                                                              7.086                                                                              4.851                                                                              1.430                                                                              7.214                             AE-DAEP          0.241                                                                              0.242                                                                              1.881                                                                              0.138                                                                              0.283                                                                              0.068                                                                              0.260                                                                              0.638                             AE-PEEDA         0.079                                                                              0.075                                                                              0.401                                                                              0.000                                                                              0.087                                                                              0.000                                                                              0.000                                                                              0.188                             iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                             AE-DPE           0.000                                                                              0.000                                                                              0.420                                                                              0.000                                                                              0.205                                                                              0.042                                                                              0.000                                                                              0.216                             BPEA             0.223                                                                              0.231                                                                              0.079                                                                              0.000                                                                              0.239                                                                              0.045                                                                              0.000                                                                              0.261                             Others           1.726                                                                              1.594                                                                              11.423                                                                             0.487                                                                              1.637                                                                              0.517                                                                              0.425                                                                              2.538                             MEA conversion, %                                                                               69.01                                                                              69.88                                                                              91.52                                                                              51.10                                                                              75.61                                                                              57.80                                                                              94.97                                                                              76.78                             DETA conversion, %                                                                              25.06                                                                              26.98                                                                              49.81                                                                              21.84                                                                              28.79                                                                              23.70                                                                              6.73                                                                               32.70                             Acyclic(N4), wt. %                                                                              93.31                                                                              93.43                                                                              66.08                                                                              97.35                                                                              92.43                                                                              97.40                                                                              87.43                                                                              89.22                             Acyclic(N5), wt. %                                                                              94.36                                                                              94.30                                                                              66.22                                                                              97.52                                                                              92.46                                                                              97.75                                                                              88.40                                                                              88.31                             Σ(N5)/Σ(N4), weight ratio                                                           0.51                                                                               0.51                                                                               0.52                                                                               0.35                                                                               0.55                                                                               0.39                                                                               0.13                                                                               0.58                              Acyclic(N4)/cyclic(<=N4),                                                                       5.62                                                                               3.74                                                                               0.60                                                                               5.96                                                                               3.45                                                                               6.16                                                                               1.66                                                                               2.76                              weight ratio                                                                   __________________________________________________________________________

                                      TABLE VIII                                   __________________________________________________________________________     Example No.      92  93  94  95  96  97  98                                    Catalyst Type    H   H   H   H   H   H   H                                     __________________________________________________________________________     Catalyst weight, gm                                                                             79.56                                                                              79.56                                                                              79.56                                                                              79.56                                                                              79.56                                                                              79.56                                                                              79.56                                 Pressure, psig   602 602 603 602 602 603 603                                   Temperature, °C.                                                                         268.2                                                                              270 280 258 270 279.6                                                                              269.3                                 Time on organics, hrs.                                                                          24  4.5 29  48  72  77  96.25                                 Duration of run, hrs.                                                                           2   2   2   2   2   2   2                                     MEA SV, gmol/hr/kgcat                                                                           1.40                                                                               2.14                                                                               0.94                                                                               0.90                                                                               2.37                                                                               1.20                                                                               0.78                                  DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                  NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                  Crude product composition, wt. %                                               EDA              1.357                                                                              2.006                                                                              4.277                                                                              2.306                                                                              1.090                                                                              3.199                                                                              2.846                                 MEA              3.284                                                                              1.883                                                                              0.923                                                                              5.261                                                                              9.399                                                                              1.511                                                                              0.959                                 PIP              1.251                                                                              1.346                                                                              2.162                                                                              1.382                                                                              0.869                                                                              1.861                                                                              1.707                                 DETA             35.076                                                                             34.162                                                                             23.951                                                                             32.591                                                                             36.463                                                                             29.869                                                                             26.799                                AEEA             0.000                                                                              0.000                                                                              0.254                                                                              1.603                                                                              1.807                                                                              0.455                                                                              0.394                                 AEP              2.193                                                                              2.794                                                                              3.951                                                                              1.914                                                                              1.135                                                                              3.122                                                                              2.893                                 HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                 TAEA             2.772                                                                              3.324                                                                              1.853                                                                              2.782                                                                              2.789                                                                              2.443                                                                              2.434                                 1-TETA           17.464                                                                             21.229                                                                             13.658                                                                             16.596                                                                             14.933                                                                             15.761                                                                             14.689                                DAEP             1.240                                                                              1.560                                                                              2.447                                                                              0.995                                                                              0.521                                                                              1.740                                                                              1.700                                 PEEDA            0.891                                                                              1.074                                                                              0.289                                                                              0.699                                                                              0.388                                                                              0.125                                                                              0.247                                 DPE              0.000                                                                              0.000                                                                              0.355                                                                              0.262                                                                              0.143                                                                              0.157                                                                              0.291                                 AE-TAEA          4.199                                                                              5.092                                                                              0.220                                                                              4.454                                                                              4.587                                                                              4.487                                                                              4.743                                 1-TEPA           9.456                                                                              11.417                                                                             10.338                                                                             9.746                                                                              8.931                                                                              11.169                                                                             10.912                                AE-DAEP          0.765                                                                              0.809                                                                              0.324                                                                              0.167                                                                              0.134                                                                              0.189                                                                              0.259                                 AE-PEEDA         0.060                                                                              0.064                                                                              0.193                                                                              0.141                                                                              0.097                                                                              0.112                                                                              0.175                                 iAE-PEEDA        0.278                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                 AE-DPE           0.000                                                                              0.242                                                                              0.496                                                                              0.187                                                                              0.158                                                                              0.174                                                                              0.433                                 BPEA             0.000                                                                              0.000                                                                              0.734                                                                              0.667                                                                              0.692                                                                              0.754                                                                              0.232                                 Others           6.124                                                                              6.280                                                                              20.326                                                                             8.645                                                                              7.394                                                                              10.911                                                                             15.928                                MEA conversion, %                                                                               90.76                                                                              95.12                                                                              97.45                                                                              85.78                                                                              74.59                                                                              95.86                                                                              97.37                                 DETA conversion, %                                                                              41.33                                                                              47.41                                                                              60.62                                                                              47.66                                                                              41.42                                                                              51.33                                                                              56.29                                 Acyclic(N4), wt. %                                                                              90.47                                                                              90.31                                                                              83.39                                                                              90.83                                                                              94.39                                                                              90.00                                                                              88.44                                 Acyclic(N5), wt. %                                                                              92.53                                                                              93.67                                                                              85.81                                                                              92.43                                                                              92.59                                                                              92.72                                                                              93.44                                 Σ(N5)/Σ(N4), weight ratio                                                           0.66                                                                               0.65                                                                               0.66                                                                               0.72                                                                               0.78                                                                               0.83                                                                               0.87                                  Acyclic(N4)/cyclic(<=N4),                                                                       3.63                                                                               3.62                                                                               1.69                                                                               3.69                                                                               5.80                                                                               2.60                                                                               2.50                                  weight ratio                                                                   __________________________________________________________________________

                                      TABLE IX                                     __________________________________________________________________________                      Example No.                                                                    99  100 101 102 103 104 105 106                               __________________________________________________________________________     Catalyst Type    I   I   I   I   I   I   I   I                                 Catalyst weight, gm                                                                             78.44                                                                              78.44                                                                              78.44                                                                              78.44                                                                              78.44                                                                              78.44                                                                              78.44                                                                              78.44                             Pressure, psig   598 598 598 598 598 598 598 598                               Temperature, °C.                                                                         268.2                                                                              270 280 258 268 270 279.6                                                                              269.3                             Time on organics, hrs.                                                                          24  4   29  48  53  72  77  96.25                             Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2                                 MEA SV, gmol/hr/kgcat                                                                           2.38                                                                               3.12                                                                               3.09                                                                               3.01                                                                               3.06                                                                               2.97                                                                               2.39                                                                               3.07                              DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                              NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                              Crude product composition, wt. %                                               EDA              1.113                                                                              0.976                                                                              1.860                                                                              0.782                                                                              1.043                                                                              1.302                                                                              1.824                                                                              0.980                             MEA              10.615                                                                             12.327                                                                             5.220                                                                              14.139                                                                             10.320                                                                             9.098                                                                              6.092                                                                              8.653                             PIP              1.129                                                                              1.005                                                                              1.496                                                                              0.859                                                                              1.132                                                                              1.320                                                                              1.611                                                                              1.111                             DETA             36.799                                                                             37.931                                                                             31.746                                                                             39.773                                                                             37.334                                                                             36.528                                                                             34.990                                                                             34.182                            AEEA             1.033                                                                              1.258                                                                              0.344                                                                              1.844                                                                              1.311                                                                              1.136                                                                              0.541                                                                              1.124                             AEP              1.305                                                                              1.132                                                                              2.067                                                                              0.979                                                                              1.353                                                                              1.472                                                                              2.104                                                                              1.379                             HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                             TAEA             2.615                                                                              2.470                                                                              2.365                                                                              2.433                                                                              2.657                                                                              2.733                                                                              2.577                                                                              2.612                             1-TETA           14.292                                                                             13.515                                                                             14.587                                                                             14.440                                                                             14.597                                                                             14.582                                                                             14.930                                                                             13.465                            DAEP             0.594                                                                              0.489                                                                              1.269                                                                              0.296                                                                              0.595                                                                              0.603                                                                              1.041                                                                              0.647                             PEEDA            0.435                                                                              0.400                                                                              0.866                                                                              0.242                                                                              0.463                                                                              0.496                                                                              0.064                                                                              0.168                             DPE              0.131                                                                              0.135                                                                              0.159                                                                              0.052                                                                              0.133                                                                              0.092                                                                              0.091                                                                              0.150                             AE-TAEA          3.929                                                                              3.799                                                                              4.211                                                                              3.918                                                                              4.621                                                                              4.393                                                                              4.377                                                                              4.357                             1-TEPA           8.291                                                                              7.823                                                                              9.865                                                                              6.776                                                                              8.516                                                                              8.862                                                                              9.611                                                                              8.767                             AE-DAEP          0.503                                                                              0.527                                                                              1.032                                                                              0.400                                                                              0.502                                                                              0.089                                                                              0.121                                                                              0.177                             AE-PEEDA         0.099                                                                              0.115                                                                              0.175                                                                              0.082                                                                              0.088                                                                              0.060                                                                              0.083                                                                              0.122                             iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                             AE-DPE           0.163                                                                              0.228                                                                              0.356                                                                              0.253                                                                              0.153                                                                              0.091                                                                              0.117                                                                              0.297                             BPEA             0.610                                                                              0.599                                                                              0.845                                                                              0.412                                                                              0.618                                                                              0.748                                                                              0.798                                                                              0.729                             Others           7.223                                                                              7.030                                                                              12.137                                                                             4.048                                                                              6.784                                                                              6.715                                                                              8.479                                                                              10.461                            MEA conversion, %                                                                               71.04                                                                              66.53                                                                              86.00                                                                              61.31                                                                              72.29                                                                              75.11                                                                              83.32                                                                              76.14                             DETA conversion, %                                                                              40.33                                                                              38.80                                                                              49.40                                                                              35.32                                                                              40.42                                                                              40.60                                                                              43.06                                                                              43.99                             Acyclic(N4), wt. %                                                                              93.58                                                                              93.98                                                                              88.08                                                                              96.62                                                                              93.54                                                                              93.56                                                                              93.61                                                                              94.34                             Acyclic(N5), wt. %                                                                              89.89                                                                              88.77                                                                              85.39                                                                              90.32                                                                              90.62                                                                              93.07                                                                              92.60                                                                              90.83                             Σ(N5)/Σ(N4), weight ratio                                                           0.75                                                                               0.77                                                                               0.86                                                                               0.68                                                                               0.79                                                                               0.77                                                                               0.81                                                                               0.85                              Acyclic(N4)/cyclic(< = N4),                                                                     4.70                                                                               5.06                                                                               2.89                                                                               6.95                                                                               4.69                                                                               4.35                                                                               3.57                                                                               4.66                              weight ratio                                                                   __________________________________________________________________________

                                      TABLE X                                      __________________________________________________________________________                      Example No.                                                                    107 108 109 110 111 112 113 114 115                           __________________________________________________________________________     Catalyst Type    J   J   J   J   J   J   J   J   J                             Catalyst weight, gm                                                                             73.3                                                                               73.3                                                                               73.3                                                                               73.3                                                                               73.3                                                                               73.3                                                                               73.3                                                                               73.3                                                                               73.3                          Pressure, psig   598 603 603 605 604 604.9                                                                              604 604 604                           Temperature, °C.                                                                         274.8                                                                              274.2                                                                              280.3                                                                              261.2                                                                              271.4                                                                              261.8                                                                              180.2                                                                              269.7                                                                              269.6                         Time on organics, hrs.                                                                          6   8   26  33  50  54.5                                                                               74  98.5                                                                               100                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   1.5 1.5                           MEA SV, gmol/hr/kgcat                                                                           4.27                                                                               4.14                                                                               3.79                                                                               3.77                                                                               3.97                                                                               3.92                                                                               3.80                                                                               4.20                                                                               4.17                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              1.429                                                                              1.424                                                                              3.172                                                                              0.868                                                                              1.570                                                                              0.800                                                                              3.025                                                                              0.882                                                                              1.051                         MEA              14.429                                                                             13.943                                                                             9.322                                                                              21.725                                                                             13.285                                                                             20.998                                                                             6.949                                                                              13.400                                                                             14.889                        PIP              1.355                                                                              1.300                                                                              2.261                                                                              0.868                                                                              1.478                                                                              0.814                                                                              2.234                                                                              1.030                                                                              1.176                         DETA             47.230                                                                             42.295                                                                             39.568                                                                             53.087                                                                             43.212                                                                             52.672                                                                             42.607                                                                             43.225                                                                             47.069                        AEEA             0.550                                                                              0.512                                                                              0.197                                                                              1.245                                                                              0.599                                                                              1.274                                                                              0.098                                                                              0.676                                                                              0.823                         AEP              1.672                                                                              1.513                                                                              2.379                                                                              0.784                                                                              1.629                                                                              0.825                                                                              2.731                                                                              1.328                                                                              1.396                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.605                                                                              2.279                                                                              2.424                                                                              2.158                                                                              2.317                                                                              2.279                                                                              2.342                                                                              2.467                                                                              2.739                         1-TETA           13.001                                                                             12.670                                                                             12.814                                                                             9.683                                                                              12.889                                                                             10.389                                                                             12.621                                                                             13.828                                                                             13.069                        DAEP             0.431                                                                              0.360                                                                              0.995                                                                              0.154                                                                              0.368                                                                              0.187                                                                              1.128                                                                              0.319                                                                              0.360                         PEEDA            0.302                                                                              0.232                                                                              0.710                                                                              0.092                                                                              0.242                                                                              0.106                                                                              0.753                                                                              0.216                                                                              0.238                         DPE              0.000                                                                              0.000                                                                              0.075                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.089                                                                              0.000                                                                              0.000                         AE-TAEA          2.986                                                                              2.963                                                                              3.398                                                                              1.553                                                                              2.893                                                                              1.804                                                                              3.351                                                                              3.239                                                                              3.092                         1-TEPA           5.571                                                                              5.909                                                                              7.347                                                                              2.674                                                                              5.827                                                                              3.180                                                                              7.449                                                                              6.276                                                                              6.252                         AE-DAEP          0.181                                                                              0.442                                                                              0.599                                                                              0.000                                                                              0.449                                                                              0.000                                                                              0.673                                                                              0.454                                                                              0.145                         AE-PEEDA         0.000                                                                              0.529                                                                              0.187                                                                              0.000                                                                              0.476                                                                              0.000                                                                              0.202                                                                              0.384                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.352                                                                              0.757                                                                              0.645                                                                              0.089                                                                              0.811                                                                              0.084                                                                              0.585                                                                              0.601                                                                              0.363                         BPEA             0.223                                                                              0.550                                                                              0.560                                                                              0.093                                                                              0.574                                                                              0.076                                                                              0.109                                                                              0.674                                                                              0.300                         Others           1.202                                                                              3.012                                                                              3.419                                                                              0.547                                                                              3.170                                                                              0.521                                                                              3.655                                                                              3.060                                                                              1.300                         MEA conversion, %                                                                               61.11                                                                              61.45                                                                              74.39                                                                              42.37                                                                              63.75                                                                              43.71                                                                              81.09                                                                              63.56                                                                              60.17                         DETA conversion, %                                                                              24.34                                                                              30.49                                                                              35.40                                                                              14.85                                                                              29.93                                                                              16.08                                                                              31.11                                                                              30.14                                                                              25.17                         Acyclic(N4), wt. %                                                                              95.51                                                                              96.19                                                                              89.54                                                                              97.97                                                                              96.15                                                                              97.74                                                                              88.37                                                                              96.82                                                                              96.36                         Acyclic(N5), wt. %                                                                              91.88                                                                              79.57                                                                              84.37                                                                              95.88                                                                              79.06                                                                              96.89                                                                              87.32                                                                              81.83                                                                              92.04                         Σ(N5)/Σ(N4), weight ratio                                                           0.57                                                                               0.72                                                                               0.75                                                                               0.36                                                                               0.70                                                                               0.40                                                                               0.73                                                                               0.69                                                                               0.62                          Acyclic(N4)/cyclic(< = N4),                                                                     4.15                                                                               4.39                                                                               2.37                                                                               6.24                                                                               4.09                                                                               6.56                                                                               2.16                                                                               5.63                                                                               4.99                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XI                                     __________________________________________________________________________                      Example No.                                                                    116 117 118 119 120 121 122 123 124                           __________________________________________________________________________     Catalyst Type    K   K   K   K   K   K   K   K   K                             Catalyst weight, gm                                                                             78.4                                                                               78.4                                                                               78.4                                                                               78.4                                                                               78.4                                                                               78.4                                                                               78.4                                                                               78.4                                                                               78.4                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         269.3                                                                              269.2                                                                              279.4                                                                              258.8                                                                              269.2                                                                              259.4                                                                              279.2                                                                              268.9                                                                              269.6                         Time on organics, hrs.                                                                          23.5                                                                               27.5                                                                               47  52  71  76  95  100 120                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           3.21                                                                               3.22                                                                               3.15                                                                               3.26                                                                               3.16                                                                               3.28                                                                               2.60                                                                               3.20                                                                               2.85                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              2.011                                                                              1.726                                                                              3.400                                                                              1.045                                                                              1.704                                                                              2.927                                                                              2.694                                                                              1.875                                                                              2.016                         MEA              19.645                                                                             19.830                                                                             10.922                                                                             24.936                                                                             17.747                                                                             13.549                                                                             6.399                                                                              19.549                                                                             17.740                        PIP              1.597                                                                              1.489                                                                              2.412                                                                              0.797                                                                              1.531                                                                              2.082                                                                              2.206                                                                              1.710                                                                              1.570                         DETA             49.999                                                                             49.815                                                                             44.929                                                                             54.559                                                                             49.660                                                                             43.523                                                                             37.413                                                                             49.063                                                                             49.599                        AEEA             0.269                                                                              0.305                                                                              0.156                                                                              0.448                                                                              0.288                                                                              0.213                                                                              0.000                                                                              0.288                                                                              0.481                         AEP              1.525                                                                              1.493                                                                              2.688                                                                              0.754                                                                              1.573                                                                              3.273                                                                              2.897                                                                              1.565                                                                              1.777                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.104                                                                              2.144                                                                              2.134                                                                              1.661                                                                              2.231                                                                              4.370                                                                              1.861                                                                              2.034                                                                              2.061                         1-TETA           9.952                                                                              10.859                                                                             11.222                                                                             7.684                                                                              10.454                                                                             11.481                                                                             11.542                                                                             9.840                                                                              10.021                        DAEP             0.081                                                                              0.238                                                                              1.038                                                                              0.095                                                                              0.470                                                                              1.096                                                                              1.664                                                                              0.680                                                                              0.442                         PEEDA            0.215                                                                              0.153                                                                              0.603                                                                              0.062                                                                              0.241                                                                              0.388                                                                              1.166                                                                              0.368                                                                              0.000                         DPE              0.000                                                                              0.000                                                                              0.051                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-TAEA          0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              4.286                                                                              4.233                                                                              0.000                                                                              1.883                         1-TEPA           1.592                                                                              1.629                                                                              2.342                                                                              0.742                                                                              1.760                                                                              4.935                                                                              8.341                                                                              1.975                                                                              2.969                         AE-DAEP          0.000                                                                              0.168                                                                              0.443                                                                              0.077                                                                              0.178                                                                              0.160                                                                              1.448                                                                              0.296                                                                              0.000                         AE-PEEDA         0.160                                                                              0.000                                                                              0.095                                                                              0.000                                                                              0.069                                                                              0.000                                                                              0.614                                                                              0.000                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.066                                                                              0.073                                                                              0.204                                                                              0.051                                                                              0.268                                                                              0.089                                                                              0.503                                                                              0.000                                                                              0.000                         BPEA             0.000                                                                              0.000                                                                              0.076                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.496                                                                              0.000                                                                              0.000                         Others           3.564                                                                              3.489                                                                              6.276                                                                              2.170                                                                              3.688                                                                              1.449                                                                              6.241                                                                              2.737                                                                              0.000                         MEA conversion, %                                                                               45.57                                                                              45.47                                                                              69.23                                                                              31.62                                                                              50.63                                                                              63.79                                                                              82.59                                                                              45.48                                                                              49.85                         DETA conversion, %                                                                              17.68                                                                              18.59                                                                              24.77                                                                              11.08                                                                              17.90                                                                              30.86                                                                              39.50                                                                              18.68                                                                              16.68                         Acyclic(N4), wt. %                                                                              97.60                                                                              97.08                                                                              88.75                                                                              98.34                                                                              94.69                                                                              91.44                                                                              82.57                                                                              91.89                                                                              96.47                         Acyclic(N5), wt. %                                                                              87.57                                                                              87.12                                                                              74.10                                                                              85.31                                                                              77.39                                                                              97.37                                                                              80.42                                                                              86.95                                                                              100.00                        Σ(N5)/Σ(N4), weight ratio                                                           0.15                                                                               0.14                                                                               0.21                                                                               0.09                                                                               0.17                                                                               0.55                                                                               0.96                                                                               0.18                                                                               0.39                          Acyclic(N4)/cyclic(< = N4),                                                                     3.53                                                                               3.86                                                                               1.97                                                                               5.47                                                                               3.33                                                                               2.32                                                                               1.69                                                                               2.75                                                                               3.19                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XII                                    __________________________________________________________________________                      Example No.                                                                    125 126 127 128 129 130 131 132 133                           __________________________________________________________________________     Catalyst Type    L   L   L   L   L   L   L   L   L                             Catalyst weight, gm                                                                             73.2                                                                               73.2                                                                               73.2                                                                               73.2                                                                               73.2                                                                               73.2                                                                               73.2                                                                               73.2                                                                               73.2                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         270.1                                                                              270 280.2                                                                              259.7                                                                              270.1                                                                              259.6                                                                              280 270 270                           Time on organics, hrs.                                                                          5   7.5 26.5                                                                               31.5                                                                               49.75                                                                              54  74  77.5                                                                               80                            Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           4.58                                                                               4.67                                                                               4.05                                                                               4.77                                                                               4.61                                                                               4.82                                                                               4.51                                                                               4.47                                                                               4.60                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.979                                                                              1.000                                                                              2.216                                                                              0.524                                                                              0.877                                                                              0.472                                                                              2.124                                                                              1.229                                                                              1.025                         MEA              17.990                                                                             19.335                                                                             10.087                                                                             24.701                                                                             17.662                                                                             24.119                                                                             9.596                                                                              17.400                                                                             17.389                        PIP              0.989                                                                              0.964                                                                              1.718                                                                              0.593                                                                              0.993                                                                              0.590                                                                              1.696                                                                              1.203                                                                              1.145                         DETA             50.172                                                                             53.162                                                                             45.219                                                                             55.645                                                                             50.697                                                                             55.944                                                                             45.259                                                                             49.313                                                                             51.748                        AEEA             0.000                                                                              0.433                                                                              0.000                                                                              1.012                                                                              0.642                                                                              1.026                                                                              0.126                                                                              0.667                                                                              0.713                         AEP              1.134                                                                              1.062                                                                              2.216                                                                              0.613                                                                              1.091                                                                              0.648                                                                              2.172                                                                              1.229                                                                              1.334                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.208                                                                              2.198                                                                              2.406                                                                              1.617                                                                              2.175                                                                              1.619                                                                              2.323                                                                              2.162                                                                              2.307                         1-TETA           9.955                                                                              10.785                                                                             12.776                                                                             7.737                                                                              10.803                                                                             7.844                                                                              12.734                                                                             10.465                                                                             11.340                        DAEP             0.232                                                                              0.218                                                                              0.936                                                                              0.103                                                                              0.249                                                                              0.110                                                                              0.896                                                                              0.273                                                                              0.300                         PEEDA            0.124                                                                              0.143                                                                              0.603                                                                              0.062                                                                              0.166                                                                              0.000                                                                              0.576                                                                              0.174                                                                              0.184                         DPE              0.000                                                                              0.075                                                                              0.075                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.085                                                                              0.000                                                                              0.000                         AE-TAEA          1.588                                                                              1.180                                                                              3.177                                                                              0.735                                                                              2.054                                                                              0.826                                                                              3.277                                                                              1.942                                                                              2.255                         1-TEPA           2.656                                                                              2.775                                                                              6.758                                                                              1.190                                                                              3.841                                                                              1.534                                                                              6.807                                                                              4.191                                                                              4.651                         AE-DAEP          0.114                                                                              0.097                                                                              0.606                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.525                                                                              0.086                                                                              0.106                         AE-PEEDA         0.000                                                                              0.000                                                                              0.149                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.136                                                                              0.000                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.000                                                                              0.000                                                                              0.235                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.222                                                                              0.121                                                                              0.135                         BPEA             0.000                                                                              0.000                                                                              0.112                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.109                                                                              0.100                                                                              0.128                         Others           6.460                                                                              0.646                                                                              1.993                                                                              0.269                                                                              0.439                                                                              0.218                                                                              1.489                                                                              0.694                                                                              0.701                         MEA conversion, %                                                                               52.45                                                                              47.17                                                                              72.49                                                                              32.06                                                                              50.75                                                                              33.87                                                                              73.52                                                                              51.33                                                                              53.62                         DETA conversion, %                                                                              19.53                                                                              13.67                                                                              26.69                                                                              9.04                                                                               15.98                                                                              8.83                                                                               25.77                                                                              18.02                                                                              17.97                         Acyclic(N4), wt. %                                                                              97.15                                                                              97.30                                                                              90.39                                                                              98.27                                                                              96.90                                                                              98.85                                                                              90.62                                                                              96.58                                                                              96.57                         Acyclic(N5), wt. %                                                                              97.38                                                                              97.61                                                                              90.01                                                                              100.00                                                                             100.00                                                                             100.00                                                                             91.03                                                                              95.24                                                                              94.93                         Σ(N5)/Σ(N4), weight ratio                                                           0.35                                                                               0.30                                                                               0.66                                                                               0.20                                                                               0.44                                                                               0.25                                                                               0.67                                                                               0.49                                                                               0.51                          Acyclic(N4)/cyclic(< = N4),                                                                     4.91                                                                               5.44                                                                               2.74                                                                               6.83                                                                               5.19                                                                               7.02                                                                               2.78                                                                               4.39                                                                               4.61                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XIII                                   __________________________________________________________________________                      Example No.                                                                    134 135 136 137 138 139 140 141 142                           __________________________________________________________________________     Catalyst Type    M   M   M   M   M   M   M   M   M                             Catalyst weight, gm                                                                             76.6                                                                               76.6                                                                               76.6                                                                               76.6                                                                               76.6                                                                               76.6                                                                               76.6                                                                               76.6                                                                               76.6                          Pressure, psig   597 599 594 596 597 598 598 578 592                           Temperature, °C.                                                                         274.8                                                                              274.2                                                                              280.3                                                                              261.2                                                                              271.4                                                                              261.8                                                                              280.2                                                                              269.7                                                                              269.6                         Time on organics, hrs.                                                                          6   8   26  33  50  54.5                                                                               74  98.5                                                                               100                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   1.5 1.5                           MEA SV, gmol/hr/kgcat                                                                           3.47                                                                               3.41                                                                               3.15                                                                               3.08                                                                               3.28                                                                               3.12                                                                               3.05                                                                               3.41                                                                               3.47                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              2.061                                                                              2.011                                                                              3.148                                                                              1.184                                                                              2.307                                                                              1.307                                                                              3.298                                                                              4.426                                                                              1.702                         MEA              11.521                                                                             11.310                                                                             6.396                                                                              20.282                                                                             13.265                                                                             20.615                                                                             5.659                                                                              11.296                                                                             14.677                        PIP              1.527                                                                              1.470                                                                              2.157                                                                              0.932                                                                              1.702                                                                              0.989                                                                              2.146                                                                              3.452                                                                              1.419                         DETA             42.334                                                                             40.741                                                                             38.310                                                                             49.435                                                                             42.179                                                                             50.484                                                                             37.713                                                                             34.699                                                                             46.940                        AEEA             0.171                                                                              0.229                                                                              0.345                                                                              1.161                                                                              0.498                                                                              1.159                                                                              0.000                                                                              0.094                                                                              0.619                         AEP              2.239                                                                              2.094                                                                              3.230                                                                              0.922                                                                              1.874                                                                              0.956                                                                              3.141                                                                              5.456                                                                              1.744                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.485                                                                              2.769                                                                              2.228                                                                              2.289                                                                              2.411                                                                              2.243                                                                              1.952                                                                              1.031                                                                              2.473                         1-TETA           13.469                                                                             14.759                                                                             13.494                                                                             11.956                                                                             12.180                                                                             10.324                                                                             11.730                                                                             8.626                                                                              13.276                        DAEP             0.942                                                                              0.959                                                                              1.643                                                                              0.249                                                                              0.703                                                                              0.219                                                                              1.537                                                                              2.523                                                                              0.455                         PEEDA            0.758                                                                              0.783                                                                              1.241                                                                              0.150                                                                              0.500                                                                              0.132                                                                              1.082                                                                              1.975                                                                              0.332                         DPE              0.099                                                                              0.097                                                                              0.135                                                                              0.000                                                                              0.076                                                                              0.000                                                                              0.130                                                                              0.128                                                                              0.000                         AE-TAEA          3.476                                                                              3.863                                                                              3.743                                                                              2.042                                                                              3.220                                                                              1.844                                                                              3.286                                                                              1.977                                                                              3.025                         1-TEPA           6.876                                                                              7.762                                                                              8.263                                                                              3.497                                                                              6.138                                                                              3.258                                                                              7.403                                                                              4.058                                                                              5.508                         AE-DAEP          0.571                                                                              0.509                                                                              1.049                                                                              0.000                                                                              0.355                                                                              0.000                                                                              1.086                                                                              2.356                                                                              0.367                         AE-PEEDA         0.150                                                                              0.159                                                                              0.419                                                                              0.000                                                                              0.107                                                                              0.000                                                                              0.878                                                                              0.928                                                                              0.121                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.410                                                                              0.460                                                                              0.567                                                                              0.176                                                                              0.433                                                                              0.123                                                                              0.974                                                                              0.089                                                                              0.242                         BPEA             0.370                                                                              0.402                                                                              0.445                                                                              0.148                                                                              0.335                                                                              0.123                                                                              0.797                                                                              0.129                                                                              0.142                         Others           3.222                                                                              3.202                                                                              4.458                                                                              0.022                                                                              2.377                                                                              0.934                                                                              5.999                                                                              8.878                                                                              1.378                         MEA conversion, %                                                                               69.06                                                                              69.99                                                                              82.87                                                                              44.85                                                                              63.31                                                                              44.03                                                                              84.47                                                                              69.87                                                                              60.81                         DETA conversion, %                                                                              32.44                                                                              35.75                                                                              39.01                                                                              20.11                                                                              30.67                                                                              18.54                                                                              38.47                                                                              45.00                                                                              25.51                         Acyclic(N4), wt. %                                                                              89.87                                                                              90.50                                                                              83.90                                                                              97.28                                                                              91.94                                                                              97.28                                                                              83.27                                                                              67.62                                                                              95.24                         Acyclic(N5), wt. %                                                                              87.34                                                                              88.37                                                                              82.89                                                                              94.47                                                                              88.39                                                                              95.40                                                                              74.10                                                                              63.28                                                                              90.73                         Σ(N5)/Σ(N4), weight ratio                                                           0.67                                                                               0.68                                                                               0.77                                                                               0.40                                                                               0.67                                                                               0.41                                                                               0.88                                                                               0.67                                                                               0.57                          Acyclic(N4)/cyclic(< = N4),                                                                     2.87                                                                               3.24                                                                               1.87                                                                               6.32                                                                               3.01                                                                               5.47                                                                               1.70                                                                               0.71                                                                               3.99                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XIV                                    __________________________________________________________________________                      Example No.                                                                    143 144 145 146 147 148 149 150 151                           __________________________________________________________________________     Catalyst Type    N   N   N   N   N   N   N   N   N                             Catalyst weight, gm                                                                             77.2                                                                               77.2                                                                               77.2                                                                               77.2                                                                               77.2                                                                               77.2                                                                               77.2                                                                               77.2                                                                               77.2                          Pressure, psig   606 602 603 599 605 601.3                                                                              604 605 602                           Temperature, °C.                                                                         274.8                                                                              274.2                                                                              280.3                                                                              261.2                                                                              271.4                                                                              261.8                                                                              280.2                                                                              269.7                                                                              269.6                         Time on organics, hrs.                                                                          6   8   26  33  50  54.5                                                                               74  98.5                                                                               100                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   1.5 1.5                           MEA SV, gmol/hr/kgcat                                                                           3.66                                                                               3.28                                                                               3.32                                                                               3.12                                                                               3.38                                                                               3.23                                                                               3.28                                                                               3.68                                                                               3.71                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              4.605                                                                              3.886                                                                              5.431                                                                              1.582                                                                              3.133                                                                              1.518                                                                              5.888                                                                              2.090                                                                              2.159                         MEA              14.165                                                                             13.840                                                                             8.988                                                                              20.796                                                                             15.163                                                                             22.247                                                                             9.341                                                                              16.165                                                                             15.935                        PIP              2.743                                                                              2.486                                                                              3.003                                                                              1.044                                                                              1.960                                                                              1.001                                                                              3.051                                                                              1.333                                                                              1.433                         DETA             39.645                                                                             39.381                                                                             34.406                                                                             46.873                                                                             40.571                                                                             50.785                                                                             37.693                                                                             42.241                                                                             45.956                        AEEA             0.101                                                                              0.264                                                                              0.101                                                                              0.891                                                                              0.476                                                                              0.962                                                                              0.000                                                                              0.631                                                                              0.594                         AEP              3.421                                                                              3.180                                                                              4.196                                                                              1.218                                                                              2.294                                                                              1.114                                                                              3.834                                                                              1.851                                                                              1.880                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             1.671                                                                              1.753                                                                              1.198                                                                              1.910                                                                              2.183                                                                              2.023                                                                              1.193                                                                              2.292                                                                              2.459                         1-TETA           10.517                                                                             11.090                                                                             10.855                                                                             9.315                                                                              11.704                                                                             9.626                                                                              10.401                                                                             11.963                                                                             12.528                        DAEP             1.223                                                                              1.224                                                                              1.875                                                                              0.287                                                                              0.898                                                                              0.251                                                                              1.503                                                                              0.631                                                                              0.765                         PEEDA            1.151                                                                              1.136                                                                              1.743                                                                              0.206                                                                              0.759                                                                              0.177                                                                              1.167                                                                              0.451                                                                              0.617                         DPE              0.130                                                                              0.119                                                                              0.213                                                                              0.000                                                                              0.080                                                                              0.000                                                                              0.109                                                                              0.000                                                                              0.105                         AE-TAEA          2.230                                                                              2.468                                                                              2.555                                                                              1.718                                                                              2.775                                                                              1.629                                                                              2.507                                                                              2.873                                                                              3.183                         1-TEPA           5.038                                                                              5.654                                                                              6.324                                                                              3.175                                                                              5.413                                                                              2.702                                                                              5.290                                                                              5.112                                                                              5.477                         AE-DAEP          0.832                                                                              0.808                                                                              1.544                                                                              0.156                                                                              0.488                                                                              0.107                                                                              1.070                                                                              0.396                                                                              0.424                         AE-PEEDA         0.403                                                                              0.315                                                                              0.858                                                                              0.000                                                                              0.160                                                                              0.000                                                                              0.446                                                                              0.111                                                                              0.106                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.130                                                                              0.259                                                                              0.457                                                                              0.096                                                                              0.092                                                                              0.000                                                                              0.307                                                                              0.366                                                                              0.235                         BPEA             0.134                                                                              0.409                                                                              0.354                                                                              0.122                                                                              0.279                                                                              0.000                                                                              0.451                                                                              0.213                                                                              0.175                         Others           4.461                                                                              4.200                                                                              9.270                                                                              1.000                                                                              3.341                                                                              0.756                                                                              6.468                                                                              2.101                                                                              1.798                         MEA conversion, %                                                                               61.68                                                                              62.60                                                                              76.38                                                                              40.76                                                                              58.41                                                                              39.45                                                                              74.52                                                                              57.13                                                                              58.04                         DETA conversion, %                                                                              36.26                                                                              36.76                                                                              46.26                                                                              20.64                                                                              33.86                                                                              17.85                                                                              38.88                                                                              26.66                                                                              28.09                         Acyclic(N4), wt. %                                                                              82.96                                                                              83.82                                                                              75.88                                                                              95.80                                                                              88.88                                                                              96.46                                                                              80.67                                                                              92.94                                                                              90.97                         Acyclic(N5), wt. %                                                                              82.90                                                                              81.94                                                                              73.43                                                                              92.89                                                                              88.93                                                                              97.60                                                                              77.42                                                                              88.03                                                                              90.21                         Σ(N5)/Σ(N4), weight ratio                                                           0.60                                                                               0.65                                                                               0.76                                                                               0.45                                                                               0.59                                                                               0.37                                                                               0.70                                                                               0.59                                                                               0.58                          Acyclic(N4)/cyclic(< = N4),                                                                     1.41                                                                               1.58                                                                               1.09                                                                               4.07                                                                               2.32                                                                               4.58                                                                               1.20                                                                               3.34                                                                               3.12                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XV                                     __________________________________________________________________________                      Example No.                                                                    152 153 154 155 156 157 158 159 160                           __________________________________________________________________________     Catalyst Type    O   O   O   O   O   O   O   O   O                             Catalyst weight, gm                                                                             74.1                                                                               74.1                                                                               74.1                                                                               74.1                                                                               74.1                                                                               74.1                                                                               74.1                                                                               74.1                                                                               74.1                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         270.1                                                                              270 280.2                                                                              259.7                                                                              270.1                                                                              259.6                                                                              280 270 270                           Time on organics, hrs.                                                                          5   7.5 26.5                                                                               31.5                                                                               49.75                                                                              54  74  77.5                                                                               80                            Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           4.32                                                                               4.45                                                                               3.86                                                                               4.75                                                                               4.55                                                                               4.76                                                                               4.72                                                                               4.88                                                                               4.68                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.799                                                                              0.893                                                                              2.371                                                                              0.614                                                                              1.122                                                                              0.619                                                                              1.998                                                                              0.866                                                                              1.017                         MEA              16.923                                                                             18.142                                                                             8.959                                                                              23.814                                                                             16.116                                                                             25.054                                                                             10.110                                                                             16.161                                                                             17.198                        PIP              1.117                                                                              1.135                                                                              0.000                                                                              0.764                                                                              1.371                                                                              0.835                                                                              1.977                                                                              1.209                                                                              1.356                         DETA             50.969                                                                             52.494                                                                             43.962                                                                             55.309                                                                             48.689                                                                             54.390                                                                             47.265                                                                             50.840                                                                             51.369                        AEEA             0.000                                                                              0.655                                                                              0.113                                                                              1.240                                                                              0.695                                                                              1.219                                                                              0.126                                                                              0.812                                                                              0.802                         AEP              1.445                                                                              1.273                                                                              2.405                                                                              0.656                                                                              1.488                                                                              0.655                                                                              2.444                                                                              1.326                                                                              1.362                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.361                                                                              2.414                                                                              2.424                                                                              1.705                                                                              2.211                                                                              1.553                                                                              2.474                                                                              2.443                                                                              2.319                         1-TETA           10.806                                                                             11.071                                                                             12.003                                                                             8.100                                                                              10.604                                                                             7.390                                                                              12.128                                                                             11.857                                                                             11.027                        DAEP             0.223                                                                              0.211                                                                              1.034                                                                              0.102                                                                              0.328                                                                              0.101                                                                              0.788                                                                              0.287                                                                              0.268                         PEEDA            0.000                                                                              0.150                                                                              0.742                                                                              0.000                                                                              0.209                                                                              0.000                                                                              0.537                                                                              0.199                                                                              0.180                         DPE              0.000                                                                              0.000                                                                              0.122                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.109                                                                              0.000                                                                              0.000                         AE-TAEA          1.975                                                                              1.711                                                                              2.755                                                                              0.748                                                                              2.130                                                                              0.714                                                                              2.508                                                                              2.424                                                                              1.870                         1-TEPA           3.599                                                                              3.260                                                                              6.223                                                                              1.444                                                                              4.940                                                                              1.373                                                                              5.742                                                                              5.006                                                                              3.901                         AE-DAEP          0.249                                                                              0.000                                                                              0.609                                                                              0.000                                                                              0.099                                                                              0.000                                                                              0.378                                                                              0.000                                                                              0.000                         AE-PEEDA         0.508                                                                              0.000                                                                              0.659                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.116                                                                              0.000                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.236                                                                              0.000                                                                              0.800                                                                              0.000                                                                              0.118                                                                              0.000                                                                              0.334                                                                              0.140                                                                              0.099                         BPEA             0.164                                                                              0.000                                                                              0.533                                                                              0.000                                                                              0.126                                                                              0.000                                                                              0.204                                                                              0.121                                                                              0.116                         Others           2.605                                                                              0.440                                                                              4.535                                                                              0.205                                                                              0.635                                                                              0.218                                                                              1.962                                                                              0.607                                                                              0.694                         MEA conversion, %                                                                               54.25                                                                              50.54                                                                              75.37                                                                              34.57                                                                              54.94                                                                              30.55                                                                              72.30                                                                              56.49                                                                              53.15                         DETA conversion, %                                                                              18.10                                                                              14.95                                                                              28.17                                                                              9.69                                                                               19.10                                                                              10.39                                                                              23.03                                                                              18.65                                                                              16.84                         Acyclic(N4), wt. %                                                                              98.33                                                                              97.39                                                                              88.38                                                                              98.97                                                                              95.98                                                                              98.88                                                                              91.06                                                                              96.71                                                                              96.75                         Acyclic(N5), wt. %                                                                              82.81                                                                              100.00                                                                             77.54                                                                              100.00                                                                             95.38                                                                              100.00                                                                             88.88                                                                              96.60                                                                              96.42                         Σ(N5)/Σ(N4), weight ratio                                                           0.50                                                                               0.36                                                                               0.71                                                                               0.22                                                                               0.56                                                                               0.23                                                                               0.58                                                                               0.52                                                                               0.43                          Acyclic(N4)/cyclic(< = N4),                                                                     4.73                                                                               4.87                                                                               3.35                                                                               6.44                                                                               3.77                                                                               5.62                                                                               2.58                                                                               4.73                                                                               4.21                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XVI                                    __________________________________________________________________________                      Example No.                                                                    161 162 163 164 165 166 167 168 169                           __________________________________________________________________________     Catalyst Type    P   P   P   P   P   P   P   P   P                             Catalyst weight, gm                                                                             78.9                                                                               78.9                                                                               78.9                                                                               78.9                                                                               78.9                                                                               78.9                                                                               78.9                                                                               78.9                                                                               78.9                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         270.3                                                                              270.8                                                                              280.9                                                                              259.5                                                                              270.8                                                                              261.4                                                                              282.6                                                                              273.4                                                                              270.8                         Time on organics, hrs.                                                                          4   7   26  31  50  55  74  79  99.5                          Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           3.12                                                                               3.22                                                                               3.28                                                                               3.33                                                                               3.43                                                                               3.59                                                                               3.37                                                                               3.31                                                                               3.46                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              1.169                                                                              1.189                                                                              2.230                                                                              1.402                                                                              1.099                                                                              0.671                                                                              1.752                                                                              0.918                                                                              1.448                         MEA              15.817                                                                             15.231                                                                             6.402                                                                              28.485                                                                             16.384                                                                             22.977                                                                             5.783                                                                              12.331                                                                             15.301                        PIP              1.664                                                                              1.609                                                                              2.315                                                                              1.465                                                                              1.764                                                                              1.139                                                                              2.015                                                                              1.420                                                                              1.843                         DETA             52.256                                                                             51.487                                                                             43.212                                                                             53.634                                                                             51.751                                                                             53.055                                                                             43.336                                                                             47.964                                                                             50.154                        AEEA             0.283                                                                              0.283                                                                              0.000                                                                              1.094                                                                              0.153                                                                              0.886                                                                              0.000                                                                              0.400                                                                              0.339                         AEP              1.915                                                                              1.855                                                                              2.978                                                                              0.777                                                                              1.978                                                                              1.094                                                                              2.884                                                                              1.762                                                                              2.059                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.062                                                                              2.339                                                                              1.830                                                                              0.884                                                                              2.131                                                                              1.899                                                                              2.473                                                                              2.651                                                                              2.259                         1-TETA           11.022                                                                             11.780                                                                             12.001                                                                             6.150                                                                              11.397                                                                             9.186                                                                              13.960                                                                             13.405                                                                             11.464                        DAEP             0.337                                                                              0.328                                                                              1.290                                                                              0.078                                                                              0.299                                                                              0.126                                                                              1.238                                                                              0.389                                                                              0.381                         PEEDA            0.207                                                                              0.217                                                                              0.927                                                                              0.046                                                                              0.186                                                                              0.076                                                                              0.763                                                                              0.288                                                                              0.260                         DPE              0.000                                                                              0.000                                                                              0.251                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-TAEA          1.815                                                                              1.985                                                                              2.926                                                                              0.503                                                                              1.572                                                                              1.100                                                                              3.768                                                                              3.096                                                                              1.880                         1-TEPA           3.691                                                                              3.831                                                                              7.181                                                                              0.912                                                                              3.369                                                                              2.347                                                                              8.080                                                                              6.384                                                                              3.990                         AE-DAEP          0.243                                                                              0.116                                                                              1.511                                                                              0.121                                                                              0.213                                                                              0.276                                                                              0.809                                                                              0.295                                                                              0.138                         AE-PEEDA         0.000                                                                              0.000                                                                              0.928                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.238                                                                              0.136                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.000                                                                              0.000                                                                              1.302                                                                              0.000                                                                              0.106                                                                              0.156                                                                              0.212                                                                              0.000                                                                              0.537                         BPEA             0.000                                                                              0.000                                                                              0.709                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.505                                                                              0.127                                                                              0.377                         Others           0.459                                                                              0.872                                                                              2.746                                                                              0.399                                                                              0.607                                                                              0.361                                                                              2.423                                                                              0.974                                                                              1.252                         MEA conversion, %                                                                               56.77                                                                              58.52                                                                              82.77                                                                              22.06                                                                              55.23                                                                              37.72                                                                              84.29                                                                              66.57                                                                              58.72                         DETA conversion, %                                                                              15.12                                                                              16.67                                                                              30.89                                                                              12.79                                                                              15.96                                                                              14.53                                                                              30.04                                                                              22.72                                                                              19.59                         Acyclic(N4), wt. %                                                                              96.01                                                                              96.29                                                                              84.86                                                                              98.26                                                                              96.54                                                                              98.20                                                                              89.14                                                                              95.95                                                                              95.54                         Acyclic(N5), wt. %                                                                              95.76                                                                              98.04                                                                              69.43                                                                              92.12                                                                              93.94                                                                              88.86                                                                              87.04                                                                              94.45                                                                              84.81                         Σ(N5)/Σ(N4), weight ratio                                                           0.42                                                                               0.40                                                                               0.89                                                                               0.21                                                                               0.38                                                                               0.34                                                                               0.74                                                                               0.60                                                                               0.48                          Acyclic(N4)/cyclic(< = N4),                                                                     3.17                                                                               3.52                                                                               1.78                                                                               2.97                                                                               3.20                                                                               4.55                                                                               2.38                                                                               4.16                                                                               3.02                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XVII                                   __________________________________________________________________________                      Example No.                                                                    170 171 172 173 174 175 176 177 178                           __________________________________________________________________________     Catalyst Type    Q   Q   Q   Q   Q   Q   Q   Q   Q                             Catalyst weight, gm                                                                             75  75  75  75  75  75  75  75  75                            Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         271.8                                                                              270 280.2                                                                              260.9                                                                              270.6                                                                              261.2                                                                              281.5                                                                              270 270                           Time on organics, hrs.                                                                          5   8.5 25  30  34  49  55  76  78                            Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           4.47                                                                               4.56                                                                               4.56                                                                               4.83                                                                               4.82                                                                               4.39                                                                               4.36                                                                               4.29                                                                               4.45                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.810                                                                              0.695                                                                              1.728                                                                              0.496                                                                              1.051                                                                              0.606                                                                              2.250                                                                              1.081                                                                              1.235                         MEA              17.286                                                                             19.405                                                                             12.726                                                                             23.941                                                                             20.602                                                                             23.930                                                                             10.050                                                                             16.058                                                                             17.476                        PIP              0.000                                                                              0.893                                                                              1.726                                                                              0.691                                                                              1.246                                                                              0.771                                                                              1.912                                                                              1.336                                                                              1.440                         DETA             49.596                                                                             50.668                                                                             47.269                                                                             55.529                                                                             51.649                                                                             54.615                                                                             43.590                                                                             49.568                                                                             50.015                        AEEA             0.486                                                                              0.691                                                                              0.138                                                                              1.063                                                                              0.715                                                                              1.234                                                                              0.241                                                                              0.655                                                                              0.684                         AEP              1.371                                                                              0.938                                                                              1.974                                                                              0.669                                                                              1.231                                                                              0.731                                                                              2.221                                                                              1.449                                                                              1.413                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             2.260                                                                              2.121                                                                              2.389                                                                              1.786                                                                              2.157                                                                              1.878                                                                              2.470                                                                              2.355                                                                              2.187                         1-TETA           12.072                                                                             9.647                                                                              11.834                                                                             8.149                                                                              10.098                                                                             8.642                                                                              12.086                                                                             11.364                                                                             11.254                        DAEP             0.252                                                                              0.179                                                                              0.649                                                                              0.097                                                                              0.211                                                                              0.112                                                                              0.851                                                                              0.313                                                                              0.251                         PEEDA            0.179                                                                              0.124                                                                              0.372                                                                              0.070                                                                              0.144                                                                              0.071                                                                              0.630                                                                              0.209                                                                              0.172                         DPE              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.068                                                                              0.000                                                                              0.000                         AE-TAEA          2.502                                                                              1.504                                                                              2.751                                                                              0.826                                                                              1.555                                                                              0.937                                                                              2.780                                                                              2.257                                                                              2.015                         1-TEPA           4.580                                                                              2.966                                                                              5.577                                                                              1.450                                                                              2.954                                                                              1.689                                                                              6.099                                                                              4.795                                                                              4.114                         AE-DAEP          0.259                                                                              0.000                                                                              0.387                                                                              0.000                                                                              0.084                                                                              0.000                                                                              0.395                                                                              0.000                                                                              0.231                         AE-PEEDA         0.105                                                                              0.000                                                                              0.100                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.111                                                                              0.000                                                                              0.177                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.166                                                                              0.000                                                                              1.181                                                                              0.000                                                                              0.077                                                                              0.000                                                                              0.451                                                                              0.115                                                                              0.108                         BPEA             0.000                                                                              0.068                                                                              0.138                                                                              0.000                                                                              0.100                                                                              0.000                                                                              0.352                                                                              0.164                                                                              0.105                         Others           0.756                                                                              0.599                                                                              1.252                                                                              0.294                                                                              0.726                                                                              0.304                                                                              2.563                                                                              0.790                                                                              0.884                         MEA conversion, %                                                                               52.45                                                                              44.86                                                                              64.94                                                                              34.49                                                                              44.04                                                                              34.90                                                                              71.93                                                                              55.92                                                                              52.53                         DETA conversion, %                                                                              18.91                                                                              14.44                                                                              22.61                                                                              9.70                                                                               16.62                                                                              11.71                                                                              27.65                                                                              19.14                                                                              19.26                         Acyclic(N4), wt. %                                                                              97.08                                                                              97.48                                                                              93.30                                                                              98.35                                                                              97.19                                                                              98.29                                                                              90.39                                                                              96.33                                                                              96.95                         Acyclic(N5), wt. %                                                                              93.03                                                                              98.50                                                                              91.18                                                                              100.00                                                                             94.52                                                                              100.00                                                                             87.15                                                                              96.19                                                                              90.81                         Σ(N5)/Σ(N4), weight ratio                                                           0.52                                                                               0.38                                                                               0.60                                                                               0.23                                                                               0.38                                                                               0.25                                                                               0.63                                                                               0.51                                                                               0.49                          Acyclic(N4)/cyclic(< = N4),                                                                     7.95                                                                               5.51                                                                               3.01                                                                               6.51                                                                               4.33                                                                               6.24                                                                               2.56                                                                               4.15                                                                               4.10                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XVIII                                  __________________________________________________________________________                      Example No.                                                                    179 180 181 182 183 184 185 186 187                           __________________________________________________________________________     Catalyst Type    R   R   R   R   R   R   R   R   R                             Catalyst weight, gm                                                                             74.9                                                                               74.9                                                                               74.9                                                                               74.9                                                                               74.9                                                                               74.9                                                                               74.9                                                                               74.9                                                                               74.9                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         269.3                                                                              269.2                                                                              279.4                                                                              258.8                                                                              269.2                                                                              259.4                                                                              279.2                                                                              268.9                                                                              269.6                         Time on organics, hrs.                                                                          23.5                                                                               27.5                                                                               47  52  71  76  95  100 120                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           3.93                                                                               3.73                                                                               3.63                                                                               3.84                                                                               3.64                                                                               3.67                                                                               3.53                                                                               3.56                                                                               3.35                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.980                                                                              0.906                                                                              2.141                                                                              0.568                                                                              1.040                                                                              0.888                                                                              2.069                                                                              1.289                                                                              1.356                         MEA              20.085                                                                             19.419                                                                             12.916                                                                             27.282                                                                             20.217                                                                             25.518                                                                             12.998                                                                             22.393                                                                             20.330                        PIP              1.509                                                                              1.448                                                                              2.211                                                                              0.850                                                                              1.624                                                                              0.922                                                                              2.027                                                                              1.573                                                                              1.718                         DETA             52.434                                                                             51.557                                                                             46.545                                                                             55.689                                                                             52.087                                                                             54.254                                                                             47.895                                                                             52.707                                                                             52.473                        AEEA             0.262                                                                              0.255                                                                              0.178                                                                              0.429                                                                              0.220                                                                              0.421                                                                              0.000                                                                              0.268                                                                              0.263                         AEP              1.402                                                                              1.413                                                                              2.106                                                                              0.696                                                                              1.428                                                                              0.823                                                                              2.307                                                                              1.348                                                                              1.537                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             1.988                                                                              2.084                                                                              2.094                                                                              1.374                                                                              1.867                                                                              1.680                                                                              1.920                                                                              1.733                                                                              1.944                         1-TETA           9.493                                                                              9.950                                                                              10.311                                                                             6.413                                                                              8.947                                                                              7.890                                                                              9.728                                                                              7.823                                                                              8.760                         DAEP             0.173                                                                              0.198                                                                              0.645                                                                              0.058                                                                              0.382                                                                              0.275                                                                              0.714                                                                              0.279                                                                              0.373                         PEEDA            0.127                                                                              0.146                                                                              0.460                                                                              0.052                                                                              0.150                                                                              0.192                                                                              0.328                                                                              0.000                                                                              0.000                         DPE              0.000                                                                              0.000                                                                              0.056                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-TAEA          0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         1-TEPA           1.257                                                                              1.371                                                                              2.257                                                                              0.448                                                                              1.195                                                                              0.801                                                                              2.316                                                                              0.979                                                                              1.375                         AE-DAEP          0.000                                                                              0.292                                                                              0.334                                                                              0.000                                                                              0.091                                                                              0.104                                                                              0.624                                                                              0.000                                                                              0.000                         AE-PEEDA         0.084                                                                              0.135                                                                              0.070                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.485                                                                              0.000                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.208                                                                              0.779                                                                              1.181                                                                              0.000                                                                              0.365                                                                              0.281                                                                              0.490                                                                              0.000                                                                              0.365                         BPEA             0.000                                                                              0.000                                                                              0.287                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.631                                                                              0.000                                                                              0.000                         Others           2.920                                                                              3.097                                                                              5.689                                                                              1.582                                                                              2.587                                                                              1.652                                                                              6.070                                                                              1.507                                                                              2.305                         MEA conversion, %                                                                               44.42                                                                              46.57                                                                              63.21                                                                              25.08                                                                              43.62                                                                              30.56                                                                              63.95                                                                              36.84                                                                              43.63                         DETA conversion, %                                                                              13.76                                                                              15.69                                                                              21.21                                                                              9.11                                                                               13.68                                                                              12.26                                                                              21.06                                                                              11.65                                                                              13.54                         Acyclic(N4), wt. %                                                                              97.46                                                                              97.22                                                                              91.45                                                                              98.61                                                                              95.31                                                                              95.35                                                                              91.79                                                                              97.16                                                                              96.64                         Acyclic(N5), wt. %                                                                              81.13                                                                              53.17                                                                              72.13                                                                              100.00                                                                             72.41                                                                              67.51                                                                              50.94                                                                              100.00                                                                             79.03                         Σ(N5)/Σ(N4), weight ratio                                                           0.13                                                                               0.21                                                                               0.23                                                                               0.06                                                                               0.15                                                                               0.12                                                                               0.36                                                                               0.10                                                                               0.16                          Acyclic(N4)/cyclic(< = N4),                                                                     3.58                                                                               3.76                                                                               2.26                                                                               4.70                                                                               3.02                                                                               4.33                                                                               2.17                                                                               2.99                                                                               2.95                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XIX                                    __________________________________________________________________________                      Example No.                                                                    188 189 190 191 192 193 194 195 196                           __________________________________________________________________________     Catalyst Type    S   S   S   S   S   S   S   S   S                             Catalyst weight, gm                                                                             77.1                                                                               77.1                                                                               77.1                                                                               77.1                                                                               77.1                                                                               77.1                                                                               77.1                                                                               77.1                                                                               77.1                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         270.3                                                                              270.8                                                                              280.9                                                                              259.5                                                                              270.8                                                                              261.4                                                                              282.6                                                                              272.4                                                                              270.8                         Time on organics, hrs.                                                                          4   7   26  31  50  55  74  79  99.5                          Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           3.57                                                                               3.84                                                                               3.80                                                                               3.90                                                                               4.07                                                                               4.29                                                                               4.00                                                                               4.02                                                                               4.09                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              1.064                                                                              1.067                                                                              2.949                                                                              1.044                                                                              1.126                                                                              0.634                                                                              1.319                                                                              0.655                                                                              0.856                         MEA              19.737                                                                             20.664                                                                             15.833                                                                             33.488                                                                             22.772                                                                             28.699                                                                             10.428                                                                             16.261                                                                             18.470                        PIP              1.010                                                                              1.060                                                                              2.508                                                                              1.029                                                                              1.433                                                                              0.868                                                                              1.591                                                                              0.964                                                                              1.166                         DETA             52.528                                                                             52.478                                                                             47.832                                                                             54.061                                                                             52.460                                                                             55.001                                                                             46.963                                                                             50.475                                                                             53.782                        AEEA             0.618                                                                              0.649                                                                              0.219                                                                              0.981                                                                              0.066                                                                              1.055                                                                              0.134                                                                              0.751                                                                              0.219                         AEP              1.111                                                                              1.092                                                                              2.117                                                                              0.537                                                                              1.255                                                                              0.600                                                                              2.045                                                                              1.283                                                                              1.400                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             1.982                                                                              1.964                                                                              1.306                                                                              0.527                                                                              1.836                                                                              1.309                                                                              2.590                                                                              2.505                                                                              2.082                         1-TETA           10.911                                                                             10.012                                                                             8.857                                                                              4.302                                                                              9.388                                                                              6.368                                                                              13.545                                                                             12.661                                                                             10.355                        DAEP             0.183                                                                              0.172                                                                              0.652                                                                              0.031                                                                              0.165                                                                              0.065                                                                              0.739                                                                              0.233                                                                              0.193                         PEEDA            0.134                                                                              0.122                                                                              0.487                                                                              0.000                                                                              0.108                                                                              0.000                                                                              0.478                                                                              0.186                                                                              0.154                         DPE              0.000                                                                              0.000                                                                              0.321                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-TAEA          1.065                                                                              1.592                                                                              1.529                                                                              0.149                                                                              0.830                                                                              0.433                                                                              3.290                                                                              2.387                                                                              1.478                         1-TEPA           2.728                                                                              3.034                                                                              2.962                                                                              0.125                                                                              2.166                                                                              0.748                                                                              6.467                                                                              4.760                                                                              2.918                         AE-DAEP          0.123                                                                              0.000                                                                              0.376                                                                              0.000                                                                              0.049                                                                              0.125                                                                              0.366                                                                              0.110                                                                              0.086                         AE-PEEDA         0.000                                                                              0.000                                                                              0.218                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.142                                                                              0.198                                                                              0.600                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.151                                                                              0.105                                                                              0.000                         BPEA             0.000                                                                              0.000                                                                              0.310                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.157                                                                              0.065                                                                              0.000                         Others           0.983                                                                              0.675                                                                              2.785                                                                              0.347                                                                              1.245                                                                              0.414                                                                              1.358                                                                              0.510                                                                              1.052                         MEA conversion, %                                                                               46.25                                                                              43.91                                                                              56.39                                                                              7.91                                                                               37.98                                                                              21.73                                                                              71.61                                                                              56.02                                                                              49.81                         DETA conversion, %                                                                              14.98                                                                              15.34                                                                              21.70                                                                              11.65                                                                              15.09                                                                              10.85                                                                              24.02                                                                              18.86                                                                              13.13                         Acyclic(N4), wt. %                                                                              97.60                                                                              97.60                                                                              87.44                                                                              99.35                                                                              97.63                                                                              99.16                                                                              92.99                                                                              97.31                                                                              97.29                         Acyclic(N5), wt. %                                                                              93.48                                                                              95.89                                                                              74.91                                                                              100.00                                                                             98.39                                                                              90.46                                                                              93.53                                                                              96.24                                                                              98.09                         Σ(N5)/Σ(N4), weight ratio                                                           0.31                                                                               0.39                                                                               0.52                                                                               0.06                                                                               0.26                                                                               0.17                                                                               0.60                                                                               0.48                                                                               0.35                          Acyclic(N4)/cyclic(< = N4),                                                                     5.29                                                                               4.89                                                                               1.67                                                                               3.02                                                                               3.79                                                                               5.01                                                                               3.32                                                                               5.69                                                                               4.27                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XX                                     __________________________________________________________________________                      Example No.                                                                    197 198 199 200 201 202 203 204 205                           __________________________________________________________________________     Catalyst Type    T   T   T   T   T   T   T   T   T                             Catalyst weight, gm                                                                             89.1                                                                               89.1                                                                               89.1                                                                               89.1                                                                               89.1                                                                               89.1                                                                               89.1                                                                               89.1                                                                               89.1                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         274.4                                                                              274.4                                                                              280.9                                                                              259.8                                                                              270.6                                                                              259.9                                                                              281.6                                                                              270.4                                                                              270.4                         Time on organics, hrs.                                                                          22  26  45.5                                                                               50.5                                                                               69  74.5                                                                               95  119 120                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   1   1                             MEA SV, gmol/hr/kgcat                                                                           3.54                                                                               3.49                                                                               3.26                                                                               3.62                                                                               3.67                                                                               3.54                                                                               3.50                                                                               7.34                                                                               3.64                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              2.720                                                                              2.147                                                                              6.050                                                                              1.506                                                                              2.063                                                                              0.510                                                                              4.522                                                                              1.700                                                                              1.717                         MEA              17.172                                                                             17.646                                                                             11.090                                                                             24.376                                                                             18.880                                                                             23.711                                                                             12.670                                                                             19.091                                                                             19.532                        PIP              3.605                                                                              3.285                                                                              6.865                                                                              1.922                                                                              2.983                                                                              1.500                                                                              5.411                                                                              2.536                                                                              2.650                         DETA             45.019                                                                             47.846                                                                             36.936                                                                             51.126                                                                             46.069                                                                             60.718                                                                             38.319                                                                             46.051                                                                             46.810                        AEEA             1.105                                                                              0.896                                                                              0.266                                                                              2.671                                                                              1.310                                                                              1.103                                                                              0.484                                                                              1.774                                                                              1.241                         AEP              2.925                                                                              2.891                                                                              6.159                                                                              1.195                                                                              2.402                                                                              1.058                                                                              4.968                                                                              2.089                                                                              2.120                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             1.209                                                                              0.424                                                                              0.376                                                                              0.813                                                                              1.233                                                                              0.599                                                                              0.517                                                                              1.195                                                                              0.782                         1-TETA           10.239                                                                             10.478                                                                             8.946                                                                              8.826                                                                              10.269                                                                             6.805                                                                              9.581                                                                              9.683                                                                              9.534                         DAEP             0.772                                                                              0.760                                                                              1.868                                                                              0.178                                                                              0.640                                                                              0.127                                                                              1.531                                                                              0.559                                                                              0.548                         PEEDA            0.840                                                                              0.880                                                                              2.576                                                                              0.170                                                                              0.724                                                                              0.140                                                                              2.159                                                                              0.624                                                                              0.603                         DPE              0.041                                                                              0.054                                                                              0.072                                                                              0.000                                                                              0.086                                                                              0.000                                                                              0.101                                                                              0.052                                                                              0.032                         AE-TAEA          0.934                                                                              0.596                                                                              0.549                                                                              0.231                                                                              0.979                                                                              0.000                                                                              0.711                                                                              0.904                                                                              0.788                         1-TEPA           4.738                                                                              4.381                                                                              4.535                                                                              2.107                                                                              4.687                                                                              0.000                                                                              5.357                                                                              4.353                                                                              4.151                         AE-DAEP          0.398                                                                              0.278                                                                              1.152                                                                              0.049                                                                              0.262                                                                              0.000                                                                              0.969                                                                              0.257                                                                              0.237                         AE-PEEDA         0.126                                                                              0.129                                                                              0.254                                                                              0.000                                                                              0.115                                                                              0.000                                                                              0.235                                                                              0.109                                                                              0.104                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.000                                                                              0.000                                                                              0.047                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         BPEA             0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         Others           1.657                                                                              1.439                                                                              3.878                                                                              0.448                                                                              1.598                                                                              0.000                                                                              3.154                                                                              1.704                                                                              1.370                         MEA Conversion, %                                                                               53.55                                                                              52.50                                                                              70.19                                                                              33.82                                                                              49.12                                                                              35.88                                                                              65.36                                                                              47.50                                                                              45.94                         DETA Conversion, %                                                                              27.63                                                                              23.46                                                                              41.00                                                                              17.51                                                                              26.21                                                                              2.41                                                                               37.74                                                                              24.74                                                                              23.00                         Acyclic(N4), wt. %                                                                              87.38                                                                              86.56                                                                              67.36                                                                              96.51                                                                              88.80                                                                              96.51                                                                              72.70                                                                              89.80                                                                              89.71                         Acyclic(N5), wt. %                                                                              91.53                                                                              92.44                                                                              77.77                                                                              97.93                                                                              93.75                                                                              0.00                                                                               83.44                                                                              93.50                                                                              93.54                         Σ(N5)/Σ(N4), weight ratio                                                           0.47                                                                               0.43                                                                               0.47                                                                               0.24                                                                               0.47                                                                               0.00                                                                               0.52                                                                               0.46                                                                               0.46                          Acyclic(N4)/cyclic(< = N4),                                                                     1.40                                                                               1.39                                                                               0.53                                                                               2.78                                                                               1.68                                                                               2.61                                                                               0.71                                                                               1.86                                                                               1.73                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XXI                                    __________________________________________________________________________                      Example No.                                                                    206 207 208 209 210 211 212 213 214                           __________________________________________________________________________     Catalyst Type    U   U   U   U   U   U   U   U   U                             Catalyst weight, gm                                                                             91.7                                                                               91.7                                                                               91.7                                                                               91.7                                                                               91.7                                                                               91.7                                                                               91.7                                                                               91.7                                                                               91.7                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         268.6                                                                              268.9                                                                              278.6                                                                              259.1                                                                              268.3                                                                              258.2                                                                              278.9                                                                              269 269.6                         Time on organics, hrs.                                                                          3   22  27  51  69.5                                                                               74  93  99  116.5                         Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           1.87                                                                               2.59                                                                               2.79                                                                               2.74                                                                               2.82                                                                               2.85                                                                               2.58                                                                               2.74                                                                               2.59                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              2.183                                                                              2.188                                                                              1.770                                                                              0.548                                                                              1.020                                                                              0.597                                                                              1.940                                                                              1.065                                                                              1.184                         MEA              27.641                                                                             27.702                                                                             4.345                                                                              16.309                                                                             9.520                                                                              16.119                                                                             3.529                                                                              9.960                                                                              7.884                         PIP              0.359                                                                              0.359                                                                              1.724                                                                              0.781                                                                              1.295                                                                              0.831                                                                              1.768                                                                              1.334                                                                              1.404                         DETA             50.123                                                                             50.233                                                                             32.473                                                                             45.537                                                                             37.563                                                                             44.839                                                                             30.507                                                                             38.688                                                                             35.307                        AEEA             1.469                                                                              1.473                                                                              0.272                                                                              2.441                                                                              0.835                                                                              2.461                                                                              0.259                                                                              0.891                                                                              0.693                         AEP              0.425                                                                              0.425                                                                              2.604                                                                              0.939                                                                              1.587                                                                              0.990                                                                              2.516                                                                              1.641                                                                              1.764                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             0.540                                                                              0.541                                                                              1.884                                                                              1.758                                                                              2.057                                                                              1.894                                                                              1.864                                                                              1.979                                                                              2.025                         1-TETA           5.907                                                                              5.920                                                                              14.212                                                                             13.575                                                                             13.856                                                                             13.962                                                                             13.839                                                                             13.903                                                                             13.810                        DAEP             0.000                                                                              0.000                                                                              1.323                                                                              0.221                                                                              0.725                                                                              0.221                                                                              1.371                                                                              0.816                                                                              0.894                         PEEDA            0.077                                                                              0.077                                                                              1.066                                                                              0.195                                                                              0.561                                                                              0.189                                                                              1.056                                                                              0.588                                                                              0.667                         DPE              0.000                                                                              0.000                                                                              0.212                                                                              0.073                                                                              0.453                                                                              0.073                                                                              0.204                                                                              0.194                                                                              0.226                         AE-TAEA          0.243                                                                              0.243                                                                              3.128                                                                              1.661                                                                              2.763                                                                              1.921                                                                              3.001                                                                              2.711                                                                              2.954                         1-TEPA           0.585                                                                              0.586                                                                              9.266                                                                              4.428                                                                              7.937                                                                              4.979                                                                              9.181                                                                              7.693                                                                              8.505                         AE-DAEP          0.000                                                                              0.000                                                                              1.117                                                                              0.186                                                                              0.635                                                                              0.255                                                                              1.174                                                                              0.589                                                                              0.748                         AE-PEEDA         0.151                                                                              0.152                                                                              0.266                                                                              0.147                                                                              0.165                                                                              0.151                                                                              0.247                                                                              0.180                                                                              0.234                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.000                                                                              0.000                                                                              0.400                                                                              0.000                                                                              0.339                                                                              0.241                                                                              0.370                                                                              0.292                                                                              0.377                         BPEA             0.000                                                                              0.000                                                                              0.692                                                                              0.194                                                                              0.581                                                                              0.058                                                                              0.692                                                                              0.473                                                                              0.620                         Others           1.677                                                                              1.680                                                                              14.327                                                                             2.888                                                                              11.047                                                                             4.339                                                                              13.830                                                                             8.942                                                                              12.375                        MEA Conversion, %                                                                               20.18                                                                              20.18                                                                              88.44                                                                              54.92                                                                              74.73                                                                              56.63                                                                              90.23                                                                              73.20                                                                              78.90                         DETA Conversion, %                                                                              13.97                                                                              13.97                                                                              48.67                                                                              25.19                                                                              40.75                                                                              28.30                                                                              49.82                                                                              38.12                                                                              43.84                         Acyclic(N4), %   98.82                                                                              98.82                                                                              86.09                                                                              96.91                                                                              90.15                                                                              97.10                                                                              85.65                                                                              90.86                                                                              89.86                         Acyclic(N5), %   84.54                                                                              84.54                                                                              83.35                                                                              92.03                                                                              86.15                                                                              90.74                                                                              83.07                                                                              87.15                                                                              85.28                         Σ(N5)/Σ(N4),                                                                        0.15                                                                               0.15                                                                               0.80                                                                               0.42                                                                               0.70                                                                               0.47                                                                               0.80                                                                               0.68                                                                               0.76                          weight ratio                                                                   Acyclic(N4)/cyclic                                                                              7.50                                                                               7.50                                                                               2.32                                                                               6.94                                                                               3.44                                                                               6.91                                                                               2.27                                                                               3.47                                                                               3.20                          (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXII                                   __________________________________________________________________________                      Example No.                                                                    215 216 217 218 219 220 221 222 223                           __________________________________________________________________________     Catalyst Type    V   V   V   V   V   V   V   V   V                             Catalyst weight, gm                                                                             79.6                                                                               79.6                                                                               79.6                                                                               79.6                                                                               79.6                                                                               79.6                                                                               79.6                                                                               79.6                                                                               79.6                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         268.6                                                                              268.9                                                                              278.6                                                                              259.1                                                                              268.3                                                                              258.2                                                                              278.9                                                                              269 269.6                         Time on organics, hrs.                                                                          3   22  27  51  69.5                                                                               74  93  99  116.5                         Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           3.34                                                                               2.66                                                                               2.48                                                                               3.46                                                                               3.32                                                                               3.85                                                                               2.73                                                                               2.84                                                                               2.42                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.402                                                                              0.984                                                                              1.667                                                                              0.394                                                                              0.739                                                                              0.489                                                                              1.751                                                                              1.291                                                                              1.139                         MEA              15.275                                                                             9.355                                                                              3.835                                                                              17.705                                                                             9.833                                                                              17.982                                                                             3.544                                                                              9.828                                                                              6.948                         PIP              1.023                                                                              1.416                                                                              1.735                                                                              0.823                                                                              1.192                                                                              0.874                                                                              1.765                                                                              1.556                                                                              1.504                         DETA             45.636                                                                             38.050                                                                             30.599                                                                             46.962                                                                             37.022                                                                             46.771                                                                             30.103                                                                             39.458                                                                             33.830                        AEEA             0.563                                                                              0.635                                                                              0.229                                                                              2.288                                                                              0.818                                                                              2.437                                                                              0.237                                                                              0.909                                                                              0.647                         AEP              1.146                                                                              1.654                                                                              2.572                                                                              0.964                                                                              1.493                                                                              0.918                                                                              2.432                                                                              1.661                                                                              1.837                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             1.055                                                                              1.701                                                                              1.742                                                                              1.714                                                                              1.968                                                                              1.798                                                                              1.727                                                                              1.992                                                                              1.965                         1-TETA           14.353                                                                             14.398                                                                             14.401                                                                             12.742                                                                             14.026                                                                             12.801                                                                             13.949                                                                             14.704                                                                             14.368                        DAEP             0.249                                                                              0.654                                                                              1.412                                                                              0.204                                                                              0.702                                                                              0.176                                                                              1.305                                                                              0.678                                                                              0.917                         PEEDA            0.325                                                                              0.561                                                                              1.102                                                                              0.191                                                                              0.551                                                                              0.167                                                                              1.053                                                                              0.549                                                                              0.702                         DPE              0.121                                                                              0.297                                                                              0.229                                                                              0.068                                                                              0.281                                                                              0.065                                                                              0.214                                                                              0.195                                                                              0.339                         AE-TAEA          1.394                                                                              2.685                                                                              2.896                                                                              1.785                                                                              2.857                                                                              2.350                                                                              2.894                                                                              2.684                                                                              2.950                         1-TEPA           5.057                                                                              7.739                                                                              9.422                                                                              4.753                                                                              8.218                                                                              4.811                                                                              9.500                                                                              7.913                                                                              9.201                         AE-DAEP          0.509                                                                              0.622                                                                              1.153                                                                              0.165                                                                              0.574                                                                              0.183                                                                              1.120                                                                              0.446                                                                              0.733                         AE-PEEDA         0.114                                                                              0.112                                                                              0.260                                                                              0.085                                                                              0.186                                                                              0.082                                                                              0.318                                                                              0.112                                                                              0.220                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.157                                                                              0.184                                                                              0.396                                                                              0.088                                                                              0.450                                                                              0.068                                                                              0.417                                                                              0.000                                                                              0.374                         BPEA             0.332                                                                              0.572                                                                              0.676                                                                              0.225                                                                              0.581                                                                              0.214                                                                              0.673                                                                              0.443                                                                              0.631                         Others           4.749                                                                              7.940                                                                              13.943                                                                             2.415                                                                              10.748                                                                             2.214                                                                              13.837                                                                             6.329                                                                              12.335                        MEA Conversion, %                                                                               58.32                                                                              74.19                                                                              89.50                                                                              51.84                                                                              73.69                                                                              51.51                                                                              90.14                                                                              73.15                                                                              81.27                         DETA Conversion, %                                                                              26.00                                                                              37.61                                                                              50.21                                                                              24.08                                                                              41.13                                                                              25.04                                                                              50.22                                                                              35.93                                                                              45.79                         Acyclic(N4), %   95.68                                                                              91.41                                                                              85.48                                                                              96.90                                                                              91.24                                                                              97.28                                                                              85.90                                                                              92.15                                                                              89.29                         Acyclic(N5), %   85.30                                                                              87.49                                                                              83.21                                                                              92.07                                                                              86.08                                                                              92.90                                                                              83.07                                                                              91.37                                                                              86.12                         Σ(N5)/Σ(N4),                                                                        0.47                                                                               0.68                                                                               0.78                                                                               0.48                                                                               0.73                                                                               0.51                                                                               0.82                                                                               0.64                                                                               0.77                          weight ratio                                                                   Acyclic(N4)/cyclic                                                                              5.38                                                                               3.51                                                                               2.29                                                                               6.43                                                                               3.79                                                                               6.63                                                                               2.32                                                                               3.60                                                                               3.08                          (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXIII                                  __________________________________________________________________________                      Example No.                                                                    224 225 226 227 228 229 230 231 232 233                       __________________________________________________________________________     Catalyst Type    W   W   W   W   W   W   W   W   W   W                         Catalyst weight, gm                                                                             87.7                                                                               87.7                                                                               87.7                                                                               87.7                                                                               87.7                                                                               87.7                                                                               87.7                                                                               87.7                                                                               87.7                                                                               87.7                      Pressure, psig   603 596 606 600 600 600 607 600 590 600                       Temperature, °C.                                                                         269 279 260 270 270 259.6                                                                              279 270 280 270                       Time on organics, hrs.                                                                          21  28  49  54  73.5                                                                               97.5                                                                               116 121 139 144                       Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           0.91                                                                               0.59                                                                               2.75                                                                               1.43                                                                               2.59                                                                               2.77                                                                               2.41                                                                               2.60                                                                               2.29                                                                               2.43                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              2.350                                                                              1.919                                                                              0.622                                                                              0.752                                                                              0.640                                                                              0.391                                                                              1.122                                                                              0.738                                                                              1.310                                                                              1.032                     MEA              23.993                                                                             22.805                                                                             29.044                                                                             27.951                                                                             26.940                                                                             30.561                                                                             23.577                                                                             28.244                                                                             22.626                                                                             14.670                    PIP              0.625                                                                              0.683                                                                              0.215                                                                              0.276                                                                              0.295                                                                              0.203                                                                              0.700                                                                              0.146                                                                              0.834                                                                              1.073                     DETA             52.709                                                                             52.718                                                                             55.792                                                                             52.407                                                                             51.421                                                                             56.953                                                                             49.965                                                                             55.022                                                                             49.613                                                                             43.078                    AEEA             0.839                                                                              0.906                                                                              0.676                                                                              0.848                                                                              0.865                                                                              0.965                                                                              0.936                                                                              1.077                                                                              0.953                                                                              1.870                     AEP              0.670                                                                              0.712                                                                              0.316                                                                              0.322                                                                              0.328                                                                              0.257                                                                              0.586                                                                              0.387                                                                              0.639                                                                              1.002                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             1.188                                                                              1.399                                                                              0.875                                                                              0.858                                                                              0.973                                                                              0.696                                                                              1.543                                                                              1.161                                                                              1.716                                                                              2.408                     1-TETA           5.320                                                                              6.386                                                                              4.275                                                                              4.119                                                                              4.573                                                                              3.717                                                                              7.655                                                                              5.591                                                                              8.550                                                                              11.687                    DAEP             0.347                                                                              0.266                                                                              0.123                                                                              0.104                                                                              0.092                                                                              0.061                                                                              0.191                                                                              0.106                                                                              0.224                                                                              0.280                     PEEDA            0.057                                                                              0.170                                                                              0.083                                                                              0.060                                                                              0.058                                                                              0.038                                                                              0.023                                                                              0.067                                                                              0.028                                                                              0.239                     DPE              0.083                                                                              0.083                                                                              0.030                                                                              0.034                                                                              0.035                                                                              0.027                                                                              0.067                                                                              0.045                                                                              0.075                                                                              0.094                     AE-TAEA          0.899                                                                              0.988                                                                              0.607                                                                              0.509                                                                              0.572                                                                              0.374                                                                              0.052                                                                              0.789                                                                              1.664                                                                              3.061                     1-TEPA           1.485                                                                              1.792                                                                              1.076                                                                              0.867                                                                              0.939                                                                              0.666                                                                              2.604                                                                              1.419                                                                              3.031                                                                              5.965                     AE-DAEP          0.280                                                                              0.202                                                                              0.116                                                                              0.085                                                                              0.000                                                                              0.035                                                                              0.142                                                                              0.084                                                                              0.162                                                                              0.312                     AE-PEEDA         0.108                                                                              0.080                                                                              0.000                                                                              0.033                                                                              0.069                                                                              0.000                                                                              0.000                                                                              0.035                                                                              0.042                                                                              0.048                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.043                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.146                     BPEA             0.107                                                                              0.106                                                                              0.059                                                                              0.022                                                                              0.081                                                                              0.000                                                                              0.175                                                                              0.080                                                                              0.210                                                                              0.374                     Others           2.935                                                                              3.026                                                                              0.992                                                                              0.725                                                                              0.939                                                                              0.685                                                                              3.151                                                                              0.949                                                                              2.575                                                                              3.282                     MEA Conversion, %                                                                               33.53                                                                              37.20                                                                              19.34                                                                              18.02                                                                              20.14                                                                              15.44                                                                              33.80                                                                              22.92                                                                              37.97                                                                              59.15                     DETA Conversion, %                                                                              13.21                                                                              13.72                                                                              7.91                                                                               8.64                                                                               9.40                                                                               6.34                                                                               16.63                                                                              10.76                                                                              19.16                                                                              28.71                     Acyclic(N4), %   93.03                                                                              93.76                                                                              95.63                                                                              96.18                                                                              96.79                                                                              97.22                                                                              97.03                                                                              96.87                                                                              96.92                                                                              95.83                     Acyclic(N5), %   81.55                                                                              87.74                                                                              90.59                                                                              90.79                                                                              90.93                                                                              96.73                                                                              89.33                                                                              91.76                                                                              91.91                                                                              91.11                     Σ(N5)/Σ(N4),                                                                        0.42                                                                               0.38                                                                               0.34                                                                               0.29                                                                               0.29                                                                               0.24                                                                               0.31                                                                               0.35                                                                               0.48                                                                               0.67                      weight ratio                                                                   Acyclic(N4)/cyclic                                                                              3.65                                                                               4.07                                                                               6.72                                                                               6.26                                                                               6.87                                                                               7.52                                                                               5.87                                                                               6.61                                                                               5.71                                                                               5.24                      (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXIV                                   __________________________________________________________________________                      Example No.                                                                    234 235 236 237 238 239 240 241 242 243                       __________________________________________________________________________     Catalyst Type    X   X   X   X   X   X   X   X   X   X                         Catalyst weight, gm                                                                             83.01                                                                              83.01                                                                              83.01                                                                              83.01                                                                              83.01                                                                              83.01                                                                              83.01                                                                              83.01                                                                              83.01                                                                              83.01                     Pressure, psig   603 596 599 599 601 597 603 603 602 603                       Temperature, °C.                                                                         271 278 260 271 260 280 270 280 270 270                       Time on organics, hrs.                                                                          99  104 123 128 147 152 171 176 195 206.75                    MEA SV, gmol/hr/kgcat                                                                           3.13                                                                               3.33                                                                               3.26                                                                               3.20                                                                               3.18                                                                               3.07                                                                               2.34                                                                               2.47                                                                               2.21                                                                               2.35                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt %                                                EDA              1.984                                                                              2.995                                                                              1.212                                                                              1.766                                                                              1.149                                                                              2.885                                                                              1.710                                                                              2.748                                                                              1.423                                                                              1.500                     MEA              6.383                                                                              3.073                                                                              13.003                                                                             5.647                                                                              11.598                                                                             3.611                                                                              10.193                                                                             5.664                                                                              10.816                                                                             11.721                    PIP              1.434                                                                              1.763                                                                              1.183                                                                              1.449                                                                              1.142                                                                              1.861                                                                              1.330                                                                              1.727                                                                              1.168                                                                              1.186                     DETA             32.000                                                                             30.373                                                                             38.190                                                                             32.197                                                                             37.489                                                                             30.866                                                                             31.155                                                                             29.136                                                                             31.286                                                                             32.092                    AEEA             0.501                                                                              0.186                                                                              1.296                                                                              0.439                                                                              1.265                                                                              0.220                                                                              0.847                                                                              0.403                                                                              0.987                                                                              1.078                     AEP              1.636                                                                              2.525                                                                              1.050                                                                              1.785                                                                              1.133                                                                              2.307                                                                              1.524                                                                              2.483                                                                              1.278                                                                              1.244                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             2.376                                                                              1.934                                                                              2.312                                                                              2.434                                                                              2.613                                                                              2.044                                                                              2.151                                                                              1.797                                                                              2.071                                                                              2.140                     1-TETA           12.940                                                                             12.003                                                                             11.840                                                                             13.576                                                                             13.452                                                                             12.217                                                                             10.663                                                                             10.795                                                                             10.563                                                                             10.796                    DAEP             0.920                                                                              1.655                                                                              0.439                                                                              1.079                                                                              0.545                                                                              1.534                                                                              0.822                                                                              1.573                                                                              0.617                                                                              0.608                     PEEDA            0.665                                                                              1.233                                                                              0.355                                                                              0.842                                                                              0.415                                                                              1.110                                                                              0.628                                                                              1.133                                                                              0.479                                                                              0.498                     DPE              0.287                                                                              0.120                                                                              0.230                                                                              0.316                                                                              0.181                                                                              0.104                                                                              0.063                                                                              0.089                                                                              0.229                                                                              0.044                     AE-TAEA          4.489                                                                              3.831                                                                              3.705                                                                              4.743                                                                              4.293                                                                              4.176                                                                              3.815                                                                              3.271                                                                              3.526                                                                              3.575                     1-TEPA           9.472                                                                              9.488                                                                              7.999                                                                              10.201                                                                             8.828                                                                              9.980                                                                              8.349                                                                              8.770                                                                              7.873                                                                              7.613                     AE-DAEP          0.811                                                                              1.698                                                                              0.463                                                                              0.927                                                                              0.392                                                                              1.458                                                                              0.759                                                                              1.596                                                                              0.624                                                                              0.664                     AE-PEEDA         0.148                                                                              0.223                                                                              0.123                                                                              0.165                                                                              0.067                                                                              0.216                                                                              0.150                                                                              0.128                                                                              0.081                                                                              0.078                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.151                                                                              0.482                                                                              0.201                                                                              0.162                                                                              0.057                                                                              0.283                                                                              0.193                                                                              0.229                                                                              0.390                                                                              0.325                     BPEA             0.149                                                                              0.853                                                                              0.178                                                                              0.215                                                                              0.057                                                                              0.232                                                                              0.082                                                                              0.655                                                                              0.601                                                                              0.569                     Others           9.595                                                                              14.536                                                                             7.200                                                                              10.480                                                                             6.385                                                                              12.915                                                                             9.485                                                                              10.732                                                                             7.587                                                                              7.371                     MEA Conversion, %                                                                               81.81                                                                              91.66                                                                              64.27                                                                              84.42                                                                              68.27                                                                              90.05                                                                              69.91                                                                              83.37                                                                              67.11                                                                              64.89                     DETA Conversion, %                                                                              45.79                                                                              51.02                                                                              37.63                                                                              47.22                                                                              39.06                                                                              49.48                                                                              45.34                                                                              49.17                                                                              43.45                                                                              42.86                     Acyclic(N4), %   89.11                                                                              82.25                                                                              93.25                                                                              87.74                                                                              93.37                                                                              83.84                                                                              89.43                                                                              81.83                                                                              90.51                                                                              91.84                     Acyclic(N5), %   91.73                                                                              80.36                                                                              92.38                                                                              91.05                                                                              95.82                                                                              86.60                                                                              91.13                                                                              82.19                                                                              87.05                                                                              87.25                     Σ(N5)/Σ(N4),                                                                        0.89                                                                               0.98                                                                               0.83                                                                               0.90                                                                               0.80                                                                               0.96                                                                               0.93                                                                               0.95                                                                               0.94                                                                               0.91                      weight ratio                                                                   Acyclic(N4)/cyclic                                                                              3.10                                                                               1.91                                                                               4.34                                                                               2.93                                                                               4.70                                                                               2.06                                                                               2.93                                                                               1.80                                                                               3.35                                                                               3.61                      (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXV                                    __________________________________________________________________________                      Example No.                                                                    244 245 246 247 248 249 250 251 252  253 254                  __________________________________________________________________________     Catalyst Type    Y   Y   Y   Y   Y   Y   Y   Y   Y    Y   Y                    Catalyst weight, gm                                                                             84.9                                                                               84.9                                                                               84.9                                                                               84.9                                                                               82.11                                                                              84.9                                                                               84.9                                                                               84.9                                                                               84.9 84.9                                                                               84.9                 Pressure, psig   604 604 604 604 602 604 602 603 600  600 600                  Temperature, °C.                                                                         268 279 258 270 259 278 269 278 279  270 270                  Time on organics, hrs.                                                                          24.5                                                                               27.75                                                                              47  52  71  76  95  99  118.5                                                                               139.8                                                                              141.5                Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2    1   1                    MEA SV, gmol/hr/kgcat                                                                           2.66                                                                               2.74                                                                               2.85                                                                               3.15                                                                               3.30                                                                               3.27                                                                               3.01                                                                               3.14                                                                               2.91 2.26                                                                               3.32                 DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00 1.00                                                                               1.00                 NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97 5.97                                                                               5.97                 Crude product composition, wt. %                                               EDA              0.261                                                                              0.356                                                                              0.244                                                                              0.282                                                                              0.226                                                                              0.267                                                                              0.193                                                                              0.300                                                                              0.276                                                                               0.137                                                                              0.175                MEA              32.096                                                                             31.884                                                                             33.649                                                                             33.262                                                                             34.748                                                                             33.604                                                                             35.331                                                                             34.218                                                                             33.615                                                                              33.551                                                                             33.298               PIP              0.012                                                                              0.017                                                                              0.009                                                                              0.013                                                                              0.000                                                                              0.013                                                                              0.000                                                                              0.014                                                                              0.015                                                                               0.021                                                                              0.015                DETA             53.034                                                                             52.823                                                                             55.550                                                                             57.167                                                                             58.160                                                                             57.340                                                                             58.631                                                                             55.561                                                                             55.690                                                                              57.452                                                                             57.445               AEEA             0.039                                                                              0.072                                                                              0.023                                                                              0.200                                                                              0.054                                                                              0.089                                                                              0.039                                                                              0.073                                                                              0.075                                                                               0.063                                                                              0.067                AEP              0.256                                                                              0.295                                                                              0.218                                                                              0.287                                                                              0.233                                                                              0.349                                                                              0.288                                                                              0.358                                                                              0.393                                                                               0.340                                                                              0.313                HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                TAEA             0.091                                                                              0.098                                                                              0.112                                                                              0.187                                                                              0.094                                                                              0.150                                                                              0.077                                                                              0.475                                                                              0.111                                                                               0.137                                                                              0.171                1-TETA           0.144                                                                              0.122                                                                              0.087                                                                              0.577                                                                              0.076                                                                              0.434                                                                              0.092                                                                              0.000                                                                              0.343                                                                               0.416                                                                              0.498                DAEP             0.024                                                                              0.031                                                                              0.016                                                                              0.056                                                                              0.000                                                                              0.021                                                                              0.000                                                                              0.067                                                                              0.044                                                                               0.030                                                                              0.027                PEEDA            0.194                                                                              0.074                                                                              0.183                                                                              0.037                                                                              0.211                                                                              0.152                                                                              0.077                                                                              0.082                                                                              0.052                                                                               0.036                                                                              0.034                DPE              0.069                                                                              0.085                                                                              0.053                                                                              0.027                                                                              0.094                                                                              0.065                                                                              0.061                                                                              0.044                                                                              0.047                                                                               0.082                                                                              0.055                AE-TAEA          0.000                                                                              0.037                                                                              0.000                                                                              0.045                                                                              0.000                                                                              0.085                                                                              0.052                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                1-TEPA           0.147                                                                              0.062                                                                              0.000                                                                              0.047                                                                              0.000                                                                              0.068                                                                              0.000                                                                              0.036                                                                              0.061                                                                               0.000                                                                              0.071                AE-DAEP          0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.024                                                                              0.060                                                                              0.027                                                                              0.091                                                                              0.114                                                                               0.028                                                                              0.000                AE-PEEDA         0.000                                                                              0.168                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.041                                                                              0.000                                                                               0.129                                                                              0.332                iAe-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                AE-DPE           0.000                                                                              0.039                                                                              0.000                                                                              0.053                                                                              0.035                                                                              0.162                                                                              0.044                                                                              0.031                                                                              0.092                                                                               0.099                                                                              0.097                BPEA             0.344                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.038                                                                              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.066                Others           1.659                                                                              2.389                                                                              1.815                                                                              2.931                                                                              1.866                                                                              3.482                                                                              2.698                                                                              3.109                                                                              3.712                                                                               2.859                                                                              2.756                MEA Conversion, %                                                                               3.06                                                                               3.91                                                                               2.16                                                                               6.89                                                                               3.11                                                                               7.25                                                                               3.34                                                                               3.38                                                                               5.38 6.32                                                                               7.15                 DETA Conversion, %                                                                              4.80                                                                               5.39                                                                               4.00                                                                               4.90                                                                               3.62                                                                               5.94                                                                               4.67                                                                               6.76                                                                               6.84 4.67                                                                               4.80                 Acyclic(N4), %   44.95                                                                              53.51                                                                              44.02                                                                              86.49                                                                              35.80                                                                              71.03                                                                              54.99                                                                              71.17                                                                              76.09                                                                               78.86                                                                              85.22                Acyclic(N5), %   30.60                                                                              32.37                                                                              0.00                                                                               63.66                                                                              0.00                                                                               37.00                                                                              42.32                                                                              18.14                                                                              22.79                                                                               0.00                                                                               12.61                Σ(N5)/Σ(N4),                                                                        0.92                                                                               0.75                                                                               0.00                                                                               0.16                                                                               0.13                                                                               0.50                                                                               0.40                                                                               0.30                                                                               0.45 0.36                                                                               0.72                 weight ratio                                                                   Acyclic(N4)/cyclic                                                                              0.42                                                                               0.44                                                                               0.41                                                                               1.82                                                                               0.32                                                                               0.97                                                                               0.40                                                                               0.84                                                                               0.82 1.09                                                                               1.51                 (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXVI                                   __________________________________________________________________________                      Example No.                                                                    255 256 257 258 259 260 261 262 263                           __________________________________________________________________________     Catalyst Type    Z   Z   Z   Z   Z   Z   Z   Z   Z                             Catalyst weight, gm                                                                             45.68                                                                              45.68                                                                              45.68                                                                              45.68                                                                              45.68                                                                              45.68                                                                              45.68                                                                              45.68                                                                              45.68                         Presure, psig    600 599 607 596 600 600 600 600 604                           Temperature, °C.                                                                         269 279 260 270 270 259.6                                                                              279 270 280                           Time on organics, hrs.                                                                          21  28  49  54  73.5                                                                               97.5                                                                               116 121 139                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           5.74                                                                               5.87                                                                               5.23                                                                               6.08                                                                               3.67                                                                               3.99                                                                               2.29                                                                               4.68                                                                               5.77                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              4.265                                                                              6.176                                                                              3.433                                                                              3.075                                                                              3.788                                                                              3.313                                                                              4.920                                                                              3.283                                                                              4.944                         MEA              5.796                                                                              3.354                                                                              10.079                                                                             7.161                                                                              8.233                                                                              12.638                                                                             5.859                                                                              8.995                                                                              7.083                         PIP              2.117                                                                              2.992                                                                              1.443                                                                              1.595                                                                              1.901                                                                              1.711                                                                              3.037                                                                              1.662                                                                              2.421                         DETA             28.085                                                                             21.574                                                                             33.585                                                                             28.671                                                                             28.468                                                                             35.387                                                                             22.837                                                                             31.649                                                                             26.907                        AEEA             0.099                                                                              0.063                                                                              0.399                                                                              0.132                                                                              0.103                                                                              0.381                                                                              0.025                                                                              0.197                                                                              0.067                         AEP              4.039                                                                              6.092                                                                              2.608                                                                              3.219                                                                              3.601                                                                              3.484                                                                              6.074                                                                              3.491                                                                              5.328                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             3.229                                                                              1.766                                                                              3.587                                                                              3.434                                                                              2.819                                                                              2.812                                                                              1.936                                                                              3.537                                                                              2.241                         1-TETA           11.677                                                                             6.932                                                                              11.244                                                                             11.553                                                                             10.261                                                                             9.480                                                                              6.501                                                                              11.947                                                                             9.241                         DAEP             2.387                                                                              3.807                                                                              1.767                                                                              1.907                                                                              1.991                                                                              1.653                                                                              4.685                                                                              2.133                                                                              3.545                         PEEDA            1.116                                                                              1.889                                                                              0.855                                                                              0.890                                                                              0.958                                                                              0.844                                                                              2.020                                                                              0.989                                                                              1.785                         DPE              0.174                                                                              0.405                                                                              0.101                                                                              0.132                                                                              0.139                                                                              0.113                                                                              0.580                                                                              0.315                                                                              0.262                         AE-TAEA          5.681                                                                              3.174                                                                              5.080                                                                              5.634                                                                              4.681                                                                              3.953                                                                              2.940                                                                              5.597                                                                              3.677                         1-TEPA           8.664                                                                              6.535                                                                              6.720                                                                              7.856                                                                              6.920                                                                              5.613                                                                              3.566                                                                              7.833                                                                              6.809                         AE-DAEP          0.935                                                                              0.738                                                                              0.803                                                                              0.708                                                                              0.722                                                                              0.579                                                                              0.757                                                                              0.823                                                                              1.937                         AE-PEEDA         0.258                                                                              1.129                                                                              0.214                                                                              0.198                                                                              0.223                                                                              0.219                                                                              0.904                                                                              0.272                                                                              0.737                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.055                                                                              0.256                                                                              0.050                                                                              0.037                                                                              0.048                                                                              0.047                                                                              0.237                                                                              0.050                                                                              0.057                         BPEA             0.975                                                                              0.822                                                                              0.665                                                                              0.847                                                                              0.688                                                                              0.813                                                                              0.350                                                                              0.801                                                                              0.858                         Others           8.808                                                                              15.412                                                                             6.548                                                                              7.053                                                                              6.595                                                                              5.262                                                                              19.371                                                                             7.036                                                                              12.602                        MEA Conversion, %                                                                               84.08                                                                              90.34                                                                              72.07                                                                              79.20                                                                              75.41                                                                              64.40                                                                              83.73                                                                              75.68                                                                              81.06                         DETA Conversion, %                                                                              54.16                                                                              63.06                                                                              44.68                                                                              50.52                                                                              49.47                                                                              40.75                                                                              62.31                                                                              49.14                                                                              57.23                         Acyclic(N4), %   80.21                                                                              58.78                                                                              84.49                                                                              83.65                                                                              80.90                                                                              82.49                                                                              53.67                                                                              81.83                                                                              67.25                         Acyclic(N5), %   86.58                                                                              76.69                                                                              87.20                                                                              88.29                                                                              87.35                                                                              85.23                                                                              74.32                                                                              87.34                                                                              74.50                         Σ(N5)/Σ(N4),                                                                        0.89                                                                               0.86                                                                               0.77                                                                               0.85                                                                               0.82                                                                               0.75                                                                               0.56                                                                               0.81                                                                               0.82                          weight ratio                                                                   Acyclic(N4)/cyclic                                                                              1.52                                                                               0.57                                                                               2.19                                                                               1.94                                                                               1.52                                                                               1.58                                                                               0.51                                                                               1.80                                                                               0.86                          (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXVII                                  __________________________________________________________________________                      Example No.                                                                    264 265 266 267 268 269 270 271 272                           __________________________________________________________________________     Catalyst Type    AA  AA  AA  AA  AA  AA  AA  AA  AA                            Catalyst weight, gm                                                                             71.9                                                                               71.9                                                                               71.9                                                                               71.9                                                                               71.9                                                                               71.9                                                                               71.9                                                                               71.9                                                                               71.9                          Pressure, psig   604 604 609 606 600 600 603 602 602                           Temperature, °C.                                                                         270 282 258 272 260 280 273 281 272                           Time on organics, hrs.                                                                          20.5                                                                               25.5                                                                               44.5                                                                               49.5                                                                               69.3                                                                               93.3                                                                               116.5                                                                              121.5                                                                              138.5                         Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           3.36                                                                               3.46                                                                               3.43                                                                               3.50                                                                               3.55                                                                               3.41                                                                               3.50                                                                               3.67                                                                               3.49                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.654                                                                              1.188                                                                              0.880                                                                              0.700                                                                              0.372                                                                              1.659                                                                              0.860                                                                              1.397                                                                              0.841                         MEA              26.367                                                                             22.170                                                                             24.384                                                                             27.194                                                                             29.909                                                                             21.016                                                                             27.518                                                                             23.168                                                                             26.560                        PIP              0.812                                                                              1.365                                                                              0.882                                                                              0.772                                                                              0.000                                                                              1.711                                                                              0.812                                                                              1.473                                                                              0.833                         DETA             51.269                                                                             45.690                                                                             48.835                                                                             51.840                                                                             55.476                                                                             43.224                                                                             51.818                                                                             46.089                                                                             52.002                        AEEA             2.016                                                                              1.702                                                                              1.570                                                                              1.900                                                                              1.779                                                                              1.481                                                                              1.827                                                                              1.619                                                                              1.976                         AEP              0.692                                                                              1.168                                                                              0.882                                                                              0.598                                                                              0.374                                                                              1.439                                                                              0.624                                                                              1.193                                                                              0.678                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             1.323                                                                              1.418                                                                              1.256                                                                              1.217                                                                              0.943                                                                              1.295                                                                              1.188                                                                              1.308                                                                              1.216                         1-TETA           7.359                                                                              8.836                                                                              7.770                                                                              6.793                                                                              5.048                                                                              8.777                                                                              6.824                                                                              8.418                                                                              7.095                         DEAP             0.163                                                                              0.347                                                                              0.300                                                                              0.112                                                                              0.071                                                                              0.485                                                                              0.130                                                                              0.370                                                                              0.143                         PEEDA            0.160                                                                              0.417                                                                              0.373                                                                              0.120                                                                              0.076                                                                              0.528                                                                              0.145                                                                              0.432                                                                              0.153                         DPE              0.046                                                                              0.069                                                                              0.061                                                                              0.042                                                                              0.025                                                                              0.114                                                                              0.046                                                                              0.034                                                                              0.050                         AE-TAEA          1.015                                                                              1.431                                                                              1.257                                                                              0.863                                                                              0.494                                                                              1.551                                                                              0.865                                                                              1.450                                                                              0.923                         1-TEPA           2.990                                                                              4.899                                                                              4.463                                                                              2.563                                                                              1.436                                                                              5.428                                                                              2.725                                                                              4.968                                                                              2.853                         AE-DAEP          0.242                                                                              0.305                                                                              0.326                                                                              0.045                                                                              0.074                                                                              0.345                                                                              0.060                                                                              0.264                                                                              0.065                         AE-PEEDA         0.106                                                                              0.077                                                                              0.079                                                                              0.000                                                                              0.000                                                                              0.094                                                                              0.062                                                                              0.187                                                                              0.038                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         BPEA             0.031                                                                              0.052                                                                              0.046                                                                              0.123                                                                              0.080                                                                              0.273                                                                              0.127                                                                              0.070                                                                              0.049                         Others           1.656                                                                              3.848                                                                              3.595                                                                              1.579                                                                              0.943                                                                              4.584                                                                              1.700                                                                              3.838                                                                              1.946                         MEA Conversion, %                                                                               29.19                                                                              40.08                                                                              35.05                                                                              26.39                                                                              18.82                                                                              42.93                                                                              26.19                                                                              38.13                                                                              28.97                         DETA Conversion, %                                                                              18.17                                                                              26.61                                                                              22.69                                                                              16.60                                                                              10.51                                                                              30.24                                                                              17.39                                                                              26.86                                                                              17.35                         Acyclic(N4), %   95.92                                                                              92.50                                                                              92.49                                                                              96.69                                                                              97.20                                                                              89.50                                                                              96.15                                                                              92.08                                                                              96.01                         Acyclic(N5), %   91.34                                                                              93.59                                                                              92.70                                                                              95.32                                                                              92.60                                                                              90.73                                                                              93.52                                                                              92.49                                                                              96.12                         Σ(N5)/Σ(N4),                                                                        0.48                                                                               0.61                                                                               0.63                                                                               0.43                                                                               0.34                                                                               0.68                                                                               0.46                                                                               0.66                                                                               0.45                          weight ratio                                                                   Acyclic(N4)/cyclic                                                                              4.64                                                                               3.05                                                                               3.61                                                                               4.87                                                                               10.96                                                                              2.33                                                                               4.56                                                                               2.78                                                                               4.48                          (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXVIII                                 __________________________________________________________________________                      Example No.                                                                    273 274 275 276 277 278 279 280 281                           __________________________________________________________________________     Catalyst Type    BB  BB  BB  BB  BB  BB  BB  BB  BB                            Catalyst weight, gm                                                                             47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                         Presure, psig    603 604 597 593 600 609 600 601 601                           Temperature, °C.                                                                         270 281 258 272 280 273 281 272 272                           Time on organics, hrs.                                                                          20.5                                                                               25.5                                                                               44.5                                                                               49.5                                                                               93.3                                                                               116.5                                                                              121.5                                                                              138.5                                                                              143.25                        Duration of run, hrs.                                                                           2   2   2   2   1   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           5.62                                                                               5.50                                                                               6.38                                                                               5.77                                                                               5.23                                                                               4.89                                                                               6.12                                                                               5.90                                                                               6.45                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              4.112                                                                              6.049                                                                              3.022                                                                              3.411                                                                              5.550                                                                              3.212                                                                              4.820                                                                              3.441                                                                              2.793                         MEA              3.993                                                                              1.805                                                                              8.392                                                                              5.992                                                                              2.263                                                                              7.178                                                                              3.892                                                                              6.533                                                                              8.131                         PIP              2.090                                                                              2.764                                                                              1.493                                                                              1.835                                                                              2.928                                                                              1.697                                                                              2.331                                                                              1.856                                                                              1.521                         DETA             26.200                                                                             19.797                                                                             30.716                                                                             29.072                                                                             19.595                                                                             30.928                                                                             25.883                                                                             27.399                                                                             32.697                        AEEA             0.105                                                                              0.029                                                                              0.466                                                                              0.193                                                                              0.059                                                                              0.257                                                                              0.082                                                                              0.253                                                                              0.337                         AEP              3.816                                                                              5.459                                                                              2.748                                                                              3.098                                                                              5.455                                                                              2.783                                                                              4.440                                                                              3.792                                                                              2.683                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             3.246                                                                              1.816                                                                              3.371                                                                              3.690                                                                              1.636                                                                              3.637                                                                              1.211                                                                              3.154                                                                              3.657                         1-TETA           12.248                                                                             7.991                                                                              11.446                                                                             12.890                                                                             7.985                                                                              12.535                                                                             9.944                                                                              11.428                                                                             12.152                        DAEP             2.327                                                                              3.836                                                                              1.908                                                                              1.821                                                                              3.625                                                                              1.607                                                                              2.852                                                                              2.506                                                                              1.457                         PEEDA            1.147                                                                              2.001                                                                              1.029                                                                              0.933                                                                              1.998                                                                              0.854                                                                              1.534                                                                              1.473                                                                              0.870                         DPE              0.205                                                                              0.259                                                                              0.072                                                                              0.159                                                                              0.343                                                                              0.212                                                                              0.287                                                                              0.292                                                                              0.199                         AE-TAEA          5.841                                                                              3.653                                                                              5.224                                                                              6.189                                                                              3.051                                                                              6.144                                                                              4.652                                                                              4.999                                                                              5.566                         1-TEPA           9.617                                                                              6.279                                                                              8.218                                                                              9.146                                                                              4.846                                                                              8.976                                                                              8.411                                                                              7.886                                                                              8.254                         AE-DAEP          1.138                                                                              2.226                                                                              1.270                                                                              0.744                                                                              0.976                                                                              0.196                                                                              0.637                                                                              0.703                                                                              0.282                         AE-PEEDA         0.133                                                                              0.798                                                                              0.566                                                                              0.032                                                                              1.236                                                                              0.237                                                                              0.789                                                                              0.817                                                                              0.091                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.198                                                                              0.335                                                                              0.262                                                                              0.062                                                                              0.124                                                                              0.064                                                                              0.176                                                                              0.106                                                                              0.138                         BPEA             0.494                                                                              1.127                                                                              0.826                                                                              0.441                                                                              0.203                                                                              1.316                                                                              1.347                                                                              1.252                                                                              1.167                         Others           13.100                                                                             17.605                                                                             11.271                                                                             10.063                                                                             19.810                                                                             9.418                                                                              16.332                                                                             12.551                                                                             9.604                         MEA Conversion, %                                                                               89.29                                                                              94.88                                                                              77.77                                                                              83.74                                                                              93.38                                                                              80.79                                                                              89.55                                                                              82.50                                                                              78.25                         DETA Conversion, %                                                                              58.24                                                                              66.61                                                                              51.64                                                                              53.13                                                                              65.93                                                                              50.81                                                                              58.69                                                                              56.38                                                                              48.01                         Acyclic(N4), %   80.81                                                                              61.67                                                                              83.12                                                                              85.06                                                                              61.73                                                                              85.82                                                                              70.48                                                                              77.35                                                                              86.22                         Acyclic(N5), %   88.73                                                                              68.89                                                                              82.14                                                                              92.30                                                                              75.68                                                                              89.29                                                                              81.59                                                                              81.74                                                                              89.16                         Σ (N5)/Σ(N4),                                                                       0.91                                                                               0.91                                                                               0.92                                                                               0.85                                                                               0.67                                                                               0.90                                                                               1.01                                                                               0.84                                                                               0.85                          weight ratio                                                                   Acyclic(N4)/cyclic                                                                              1.62                                                                               0.68                                                                               2.04                                                                               2.11                                                                               0.67                                                                               2.26                                                                               0.97                                                                               1.47                                                                               2.35                          (< = N4), weight ratio                                                         __________________________________________________________________________                      Example No.                                                                    282 283 284 285 286 287 288 289 290                           __________________________________________________________________________     Catalyst Type    BB  BB  BB  BB  BB  BB  BB  BB  BB                            Catalyst weight, gm                                                                             47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                                                                              47.15                         Pressure, psig   603 602 601 602 596 599 600 600 600                           Temperature, °C.                                                                         270 280 260 269 259 269 269 279.6                                                                              268                           Time on organics, hrs.                                                                          22.5                                                                               27.5                                                                               46.5                                                                               51.5                                                                               70.5                                                                               99.5                                                                               120 143 169.5                         Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           4.97                                                                               4.30                                                                               3.85                                                                               2.94                                                                               0.75                                                                               5.31                                                                               5.03                                                                               4.80                                                                               3.32                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              2.967                                                                              4.366                                                                              4.440                                                                              2.967                                                                              4.460                                                                              1.952                                                                              3.142                                                                              4.055                                                                              2.453                         MEA              9.344                                                                              4.942                                                                              4.115                                                                              7.299                                                                              4.769                                                                              11.879                                                                             10.054                                                                             6.454                                                                              12.691                        PIP              1.511                                                                              2.037                                                                              2.043                                                                              1.452                                                                              2.132                                                                              1.272                                                                              1.700                                                                              2.182                                                                              1.366                         DETA             31.637                                                                             26.975                                                                             25.016                                                                             30.734                                                                             25.564                                                                             38.106                                                                             32.444                                                                             26.800                                                                             38.319                        AEEA             0.424                                                                              0.162                                                                              0.130                                                                              0.465                                                                              0.229                                                                              0.767                                                                              0.506                                                                              0.183                                                                              0.649                         AEP              2.464                                                                              3.612                                                                              3.730                                                                              2.436                                                                              3.835                                                                              1.957                                                                              3.105                                                                              4.023                                                                              2.028                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             3.232                                                                              3.170                                                                              3.039                                                                              4.030                                                                              3.514                                                                              3.588                                                                              2.814                                                                              2.467                                                                              3.544                         1-TETA           11.069                                                                             12.118                                                                             12.039                                                                             13.420                                                                             13.075                                                                             11.521                                                                             10.058                                                                             9.825                                                                              12.044                        DAEP             1.231                                                                              2.138                                                                              2.332                                                                              1.243                                                                              2.045                                                                              0.861                                                                              1.515                                                                              2.269                                                                              0.889                         PEEDA            0.679                                                                              1.195                                                                              1.326                                                                              0.704                                                                              1.131                                                                              0.508                                                                              0.922                                                                              1.458                                                                              0.524                         DPE              0.187                                                                              0.300                                                                              0.338                                                                              0.255                                                                              0.476                                                                              0.141                                                                              0.254                                                                              0.309                                                                              0.124                         AE-TAEA          5.103                                                                              5.422                                                                              5.331                                                                              6.126                                                                              5.933                                                                              4.797                                                                              4.017                                                                              4.146                                                                              4.610                         1-TEPA           7.681                                                                              9.105                                                                              9.262                                                                              8.935                                                                              9.548                                                                              6.845                                                                              6.630                                                                              7.426                                                                              6.884                         AE-DAEP          0.028                                                                              0.438                                                                              0.477                                                                              0.260                                                                              0.377                                                                              0.367                                                                              0.846                                                                              1.348                                                                              0.370                         AE-PEEDA         0.645                                                                              0.119                                                                              0.143                                                                              0.119                                                                              0.141                                                                              0.096                                                                              0.119                                                                              0.616                                                                              0.106                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.437                                                                              0.190                                                                              0.276                                                                              0.126                                                                              0.050                                                                              0.048                                                                              0.028                                                                              0.092                                                                              0.029                         BPEA             0.997                                                                              0.316                                                                              0.321                                                                              0.381                                                                              0.328                                                                              0.593                                                                              0.605                                                                              0.273                                                                              0.533                         Others           6.554                                                                              13.105                                                                             14.254                                                                             9.326                                                                              11.795                                                                             5.441                                                                              9.162                                                                              13.636                                                                             4.287                         MEA Conversion, %                                                                               73.30                                                                              86.63                                                                              88.77                                                                              80.18                                                                              87.07                                                                              67.40                                                                              71.78                                                                              82.09                                                                              65.35                         DETA Conversion, %                                                                              46.27                                                                              56.62                                                                              59.43                                                                              50.41                                                                              58.82                                                                              37.84                                                                              45.87                                                                              55.81                                                                              37.82                         Acyclic(N4), %   87.21                                                                              80.80                                                                              79.05                                                                              88.79                                                                              81.96                                                                              90.91                                                                              82.71                                                                              75.29                                                                              91.03                         Acyclic(N5), %   85.85                                                                              93.18                                                                              92.31                                                                              94.44                                                                              94.53                                                                              91.34                                                                              86.95                                                                              83.25                                                                              91.71                         Σ(N5)/Σ(N4),                                                                        0.91                                                                               0.82                                                                               0.83                                                                               0.81                                                                               0.81                                                                               0.77                                                                               0.79                                                                               0.85                                                                               0.73                          weight ratio                                                                   Acyclic(N4)/cyclic                                                                              2.36                                                                               1.65                                                                               1.54                                                                               2.87                                                                               1.72                                                                               3.19                                                                               1.72                                                                               1.20                                                                               3.16                          (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXIX                                   __________________________________________________________________________                      Example No.                                                                    291 292 293 294 295 296 297 298 299 300                       __________________________________________________________________________     Catalyst Type    CC  CC  CC  CC  CC  CC  CC  CC  CC  CC                        Catalyst weight, gm                                                                             76.68                                                                              76.68                                                                              76.68                                                                              76.68                                                                              76.68                                                                              76.68                                                                              76.68                                                                              76.68                                                                              76.68                                                                              76.68                     Pressure, psig   603 603 604 604 604 604 602 600 600 603                       Temperature, °C.                                                                         270 260 269 259 280 280 269 269 279.6                                                                              268                       Time on organics, hrs.                                                                          22.5                                                                               46.5                                                                               51.5                                                                               70.5                                                                               75.5                                                                               94.5                                                                               99.5                                                                               120 143 169.5                     Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           3.56                                                                               3.18                                                                               3.05                                                                               2.39                                                                               2.57                                                                               2.86                                                                               3.10                                                                               2.58                                                                               2.14                                                                               2.10                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              1.048                                                                              1.891                                                                              1.635                                                                              0.886                                                                              2.023                                                                              1.862                                                                              0.964                                                                              1.307                                                                              2.134                                                                              1.598                     MEA              15.586                                                                             7.180                                                                              13.602                                                                             16.846                                                                             6.993                                                                              5.180                                                                              14.419                                                                             11.949                                                                             4.391                                                                              10.047                    PIP              0.813                                                                              1.493                                                                              1.323                                                                              0.749                                                                              1.617                                                                              1.560                                                                              1.056                                                                              1.181                                                                              1.690                                                                              1.287                     DETA             41.901                                                                             34.342                                                                             39.594                                                                             43.641                                                                             34.966                                                                             31.278                                                                             43.144                                                                             40.674                                                                             33.084                                                                             40.233                    AEEA             1.865                                                                              0.611                                                                              1.010                                                                              2.381                                                                              0.717                                                                              0.512                                                                              2.061                                                                              1.865                                                                              0.489                                                                              1.972                     AEP              0.823                                                                              1.517                                                                              1.156                                                                              0.704                                                                              1.562                                                                              1.651                                                                              0.963                                                                              1.108                                                                              1.845                                                                              1.344                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             2.659                                                                              2.739                                                                              2.487                                                                              2.206                                                                              2.576                                                                              2.486                                                                              2.470                                                                              2.584                                                                              2.664                                                                              2.778                     1-TETA           11.989                                                                             13.676                                                                             12.245                                                                             10.267                                                                             13.010                                                                             12.812                                                                             11.950                                                                             12.589                                                                             14.102                                                                             14.021                    DAEP             0.232                                                                              0.654                                                                              0.419                                                                              0.182                                                                              0.622                                                                              0.734                                                                              0.275                                                                              0.343                                                                              0.814                                                                              0.472                     PEEDA            0.217                                                                              0.518                                                                              0.333                                                                              0.166                                                                              0.508                                                                              0.588                                                                              0.265                                                                              0.328                                                                              0.634                                                                              0.384                     DPE              0.109                                                                              0.083                                                                              0.058                                                                              0.039                                                                              0.100                                                                              0.095                                                                              0.052                                                                              0.061                                                                              0.132                                                                              0.148                     AE-TAEA          3.022                                                                              4.382                                                                              3.620                                                                              1.989                                                                              4.314                                                                              4.182                                                                              3.097                                                                              3.397                                                                              4.800                                                                              3.528                     1-TEPA           5.378                                                                              8.807                                                                              6.947                                                                              3.856                                                                              8.743                                                                              8.887                                                                              6.071                                                                              6.875                                                                              10.097                                                                             7.285                     AE-DAEP          0.000                                                                              0.169                                                                              0.298                                                                              0.077                                                                              0.555                                                                              0.161                                                                              0.332                                                                              0.223                                                                              0.191                                                                              0.386                     AE-PEEDA         0.213                                                                              0.106                                                                              0.056                                                                              0.030                                                                              0.119                                                                              0.104                                                                              0.049                                                                              0.039                                                                              0.121                                                                              0.060                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.429                                                                              0.057                                                                              0.000                                                                              0.000                                                                              0.079                                                                              0.078                                                                              0.045                                                                              0.000                                                                              0.109                                                                              0.086                     BPEA             0.423                                                                              0.255                                                                              0.529                                                                              0.212                                                                              0.715                                                                              0.986                                                                              0.407                                                                              0.447                                                                              1.153                                                                              0.657                     Others           2.432                                                                              7.971                                                                              4.837                                                                              2.430                                                                              8.651                                                                              8.353                                                                              4.000                                                                              4.471                                                                              9.150                                                                              4.134                     MEA Conversion, %                                                                               55.76                                                                              79.54                                                                              62.13                                                                              50.35                                                                              80.43                                                                              84.46                                                                              60.32                                                                              66.53                                                                              87.79                                                                              72.35                     DETA Conversion, %                                                                              29.31                                                                              41.82                                                                              34.48                                                                              23.55                                                                              41.85                                                                              44.25                                                                              29.45                                                                              32.30                                                                              45.34                                                                              34.20                     Acyclic(N4), %   96.35                                                                              92.90                                                                              94.78                                                                              96.99                                                                              92.69                                                                              91.52                                                                              96.06                                                                              95.40                                                                              91.39                                                                              94.36                     Acyclic(N5), %   88.75                                                                              95.74                                                                              92.28                                                                              94.82                                                                              89.89                                                                              90.77                                                                              91.66                                                                              93.55                                                                              90.44                                                                              90.10                     Σ(N5)/Σ(N4),                                                                        0.62                                                                               0.78                                                                               0.74                                                                               0.48                                                                               0.86                                                                               0.86                                                                               0.67                                                                               0.69                                                                               0.90                                                                               0.67                      weight ratio                                                                   Acyclic(N4)/cyclic                                                                              6.67                                                                               3.85                                                                               4.48                                                                               6.78                                                                               3.54                                                                               3.31                                                                               5.53                                                                               5.02                                                                               3.28                                                                               4.62                      (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXX                                    __________________________________________________________________________                      Example No.                                                                    301 302 303 304 305 306 307 308 309 310                       __________________________________________________________________________     Catalyst Type    DD  DD  DD  DD  DD  DD  DD  DD  DD  DD                        Catalyst weight, gm                                                                             78.75                                                                              78.75                                                                              78.75                                                                              78.75                                                                              78.75                                                                              78.75                                                                              78.75                                                                              78.75                                                                              78.75                                                                              78.75                     Pressure, psig   598 598 599 598 600 600 598 600 598 600                       Temperature, °C.                                                                         269 279 260 270 270 259.6                                                                              279 270 280 270                       Time on organics, hrs.                                                                          21  28  49  54  73.5                                                                               97.5                                                                               116 121 139 144                       Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           2.92                                                                               2.87                                                                               3.06                                                                               2.85                                                                               2.60                                                                               2.98                                                                               2.80                                                                               2.99                                                                               2.81                                                                               2.96                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              1.555                                                                              1.668                                                                              1.004                                                                              0.978                                                                              0.998                                                                              0.533                                                                              2.192                                                                              1.116                                                                              1.691                                                                              0.974                     MEA              15.132                                                                             10.654                                                                             18.325                                                                             16.432                                                                             15.110                                                                             22.024                                                                             8.483                                                                              16.234                                                                             7.965                                                                              14.943                    PIP              0.978                                                                              1.343                                                                              0.749                                                                              0.856                                                                              0.926                                                                              0.581                                                                              1.662                                                                              1.112                                                                              1.577                                                                              1.057                     DETA             41.054                                                                             38.593                                                                             44.607                                                                             43.072                                                                             41.241                                                                             51.032                                                                             35.320                                                                             45.272                                                                             36.976                                                                             44.374                    AEEA             1.683                                                                              0.873                                                                              1.751                                                                              1.997                                                                              1.834                                                                              2.629                                                                              0.512                                                                              1.883                                                                              0.650                                                                              1.955                     AEP              1.101                                                                              1.347                                                                              0.771                                                                              0.821                                                                              0.835                                                                              0.570                                                                              1.905                                                                              0.982                                                                              1.561                                                                              1.000                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             2.712                                                                              2.489                                                                              2.232                                                                              2.241                                                                              2.226                                                                              1.861                                                                              2.166                                                                              2.390                                                                              2.589                                                                              2.511                     1-TETA           11.777                                                                             11.906                                                                             10.383                                                                             10.387                                                                             10.429                                                                             8.845                                                                              11.724                                                                             11.589                                                                             13.232                                                                             12.136                    DAEP             0.423                                                                              0.486                                                                              0.280                                                                              0.215                                                                              0.235                                                                              0.126                                                                              0.995                                                                              0.266                                                                              0.649                                                                              0.285                     PEEDA            0.327                                                                              0.415                                                                              0.253                                                                              0.183                                                                              0.199                                                                              0.101                                                                              0.736                                                                              0.226                                                                              0.512                                                                              0.249                     DPE              0.088                                                                              0.183                                                                              0.098                                                                              0.092                                                                              0.091                                                                              0.057                                                                              0.262                                                                              0.089                                                                              0.219                                                                              0.098                     AE-TAEA          3.411                                                                              3.691                                                                              2.918                                                                              2.501                                                                              2.621                                                                              1.429                                                                              3.662                                                                              3.017                                                                              4.503                                                                              3.121                     1-TEPA           6.041                                                                              6.960                                                                              5.789                                                                              4.661                                                                              4.999                                                                              2.823                                                                              8.129                                                                              5.730                                                                              9.114                                                                              6.079                     AE-DAEP          0.397                                                                              0.339                                                                              0.351                                                                              0.199                                                                              0.231                                                                              0.053                                                                              1.154                                                                              0.242                                                                              0.570                                                                              0.278                     AE-PEEDA         0.058                                                                              0.077                                                                              0.059                                                                              0.052                                                                              0.032                                                                              0.000                                                                              0.223                                                                              0.032                                                                              0.163                                                                              0.042                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.052                                                                              0.153                                                                              0.049                                                                              0.072                                                                              0.067                                                                              0.000                                                                              0.208                                                                              0.077                                                                              0.070                                                                              0.097                     BPEA             0.695                                                                              0.772                                                                              0.603                                                                              0.425                                                                              0.457                                                                              0.177                                                                              0.094                                                                              0.547                                                                              0.803                                                                              0.556                     Others           4.145                                                                              4.991                                                                              3.687                                                                              2.354                                                                              2.636                                                                              1.310                                                                              9.047                                                                              2.757                                                                              7.406                                                                              3.016                     MEA Conversion, %                                                                               58.37                                                                              69.49                                                                              50.38                                                                              52.25                                                                              55.02                                                                              39.54                                                                              76.37                                                                              56.07                                                                              78.27                                                                              59.37                     DETA Conversion, %                                                                              32.88                                                                              34.31                                                                              28.22                                                                              25.62                                                                              27.04                                                                              16.74                                                                              41.52                                                                              27.19                                                                              40.06                                                                              28.29                     Acyclic(N4), %   94.53                                                                              92.99                                                                              95.23                                                                              96.26                                                                              96.01                                                                              97.42                                                                              87.46                                                                              96.01                                                                              91.98                                                                              95.86                     Acyclic(N5), %   88.72                                                                              88.82                                                                              89.13                                                                              90.54                                                                              90.63                                                                              94.86                                                                              87.54                                                                              90.69                                                                              89.45                                                                              90.43                     Σ(N5)/Σ(N4),                                                                        0.70                                                                               0.77                                                                               0.74                                                                               0.60                                                                               0.64                                                                               0.41                                                                               0.85                                                                               0.66                                                                               0.88                                                                               0.67                      weight ratio                                                                   Acyclic(N4)/cyclic                                                                              4.97                                                                               3.81                                                                               5.86                                                                               5.83                                                                               5.53                                                                               7.46                                                                               2.50                                                                               5.23                                                                               3.50                                                                               5.45                      (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXXI                                   __________________________________________________________________________                      Example No.                                                                    311 312 313 314 315 316 317 318 319 320                       __________________________________________________________________________     Catalyst Type    EE  EE  EE  EE  EE  EE  EE  EE  EE  EE                        Catalyst weight, gm                                                                             76.67                                                                              76.67                                                                              76.67                                                                              76.67                                                                              76.67                                                                              76.67                                                                              76.67                                                                              76.67                                                                              76.67                                                                              76.67                     Pressure, psig   599 599 609 599 600 598 596 598 600 599                       Temperature, °C.                                                                         270 280 260 269 259 280 280 269 269 268                       Time on organics, hrs.                                                                          22.5                                                                               27.5                                                                               46.5                                                                               51.5                                                                               70.5                                                                               75.5                                                                               94.5                                                                               99.5                                                                               120 169.5                     Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           3.05                                                                               3.06                                                                               2.79                                                                               3.10                                                                               3.07                                                                               3.13                                                                               3.03                                                                               3.01                                                                               3.05                                                                               3.15                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              1.520                                                                              2.437                                                                              2.447                                                                              1.228                                                                              1.029                                                                              2.414                                                                              2.547                                                                              1.320                                                                              1.437                                                                              1.242                     MEA              14.652                                                                             8.505                                                                              6.424                                                                              13.718                                                                             18.262                                                                             7.632                                                                              6.416                                                                              14.174                                                                             12.516                                                                             13.988                    PIP              1.110                                                                              1.615                                                                              1.625                                                                              1.089                                                                              0.811                                                                              1.685                                                                              1.788                                                                              1.154                                                                              1.228                                                                              1.100                     DETA             39.856                                                                             33.953                                                                             30.620                                                                             42.604                                                                             44.433                                                                             34.076                                                                             32.533                                                                             40.980                                                                             39.040                                                                             42.773                    AEEA             1.060                                                                              0.447                                                                              0.314                                                                              1.855                                                                              1.945                                                                              0.437                                                                              0.334                                                                              1.170                                                                              1.071                                                                              1.048                     AEP              1.075                                                                              1.737                                                                              1.834                                                                              1.025                                                                              0.733                                                                              1.846                                                                              2.086                                                                              1.119                                                                              1.173                                                                              1.187                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             2.436                                                                              2.526                                                                              2.311                                                                              2.830                                                                              2.495                                                                              2.424                                                                              2.285                                                                              2.594                                                                              2.614                                                                              2.592                     1-TETA           11.953                                                                             13.615                                                                             12.962                                                                             13.423                                                                             11.709                                                                             13.253                                                                             12.977                                                                             12.761                                                                             12.998                                                                             14.044                    DAEP             0.316                                                                              0.845                                                                              0.960                                                                              0.297                                                                              0.197                                                                              0.863                                                                              1.049                                                                              0.408                                                                              0.461                                                                              0.325                     PEEDA            0.271                                                                              0.647                                                                              0.738                                                                              0.284                                                                              0.177                                                                              0.663                                                                              0.796                                                                              0.337                                                                              0.392                                                                              0.267                     DPE              0.114                                                                              0.099                                                                              0.099                                                                              0.049                                                                              0.040                                                                              0.099                                                                              0.102                                                                              0.071                                                                              0.074                                                                              0.052                     AE-TAEA          3.524                                                                              4.505                                                                              4.333                                                                              3.359                                                                              2.704                                                                              4.359                                                                              4.387                                                                              3.710                                                                              3.897                                                                              3.401                     1-TEPA           6.384                                                                              9.138                                                                              9.198                                                                              6.628                                                                              5.017                                                                              9.080                                                                              9.494                                                                              6.780                                                                              7.415                                                                              6.586                     AE-DAEP          0.000                                                                              0.248                                                                              0.279                                                                              0.314                                                                              0.207                                                                              0.679                                                                              0.267                                                                              0.307                                                                              0.269                                                                              0.300                     AE-PEEDA         0.229                                                                              0.135                                                                              0.140                                                                              0.042                                                                              0.063                                                                              0.126                                                                              0.123                                                                              0.032                                                                              0.057                                                                              0.054                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.553                                                                              0.191                                                                              0.210                                                                              0.000                                                                              0.000                                                                              0.052                                                                              0.093                                                                              0.000                                                                              0.033                                                                              0.000                     BPEA             0.522                                                                              0.338                                                                              0.365                                                                              0.442                                                                              0.300                                                                              0.794                                                                              0.831                                                                              0.530                                                                              0.577                                                                              0.532                     Others           3.075                                                                              9.229                                                                              10.383                                                                             4.003                                                                              2.618                                                                              9.258                                                                              10.540                                                                             4.653                                                                              5.267                                                                              2.788                     MEA Conversion, %                                                                               58.39                                                                              76.75                                                                              81.53                                                                              63.00                                                                              49.80                                                                              79.10                                                                              82.29                                                                              61.34                                                                              65.43                                                                              62.89                     DETA Conversion, %                                                                              32.73                                                                              44.85                                                                              47.68                                                                              31.70                                                                              27.42                                                                              44.55                                                                              46.62                                                                              33.56                                                                              35.92                                                                              30.74                     Acyclic(N4), %   95.36                                                                              91.03                                                                              89.48                                                                              96.26                                                                              97.17                                                                              90.61                                                                              88.68                                                                              94.65                                                                              94.40                                                                              96.27                     Acyclic(N5), %   88.37                                                                              93.73                                                                              93.16                                                                              92.61                                                                              93.12                                                                              89.06                                                                              91.35                                                                              92.35                                                                              92.35                                                                              91.85                     Σ(N5)/Σ(N4),                                                                        0.74                                                                               0.82                                                                               0.85                                                                               0.64                                                                               0.57                                                                               0.87                                                                               0.88                                                                               0.70                                                                               0.74                                                                               0.63                      weight ratio                                                                   Acyclic(N4)/cyclic                                                                              4.99                                                                               3.27                                                                               2.91                                                                               5.92                                                                               7.25                                                                               3.04                                                                               2.62                                                                               4.97                                                                               4.69                                                                               5.68                      (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXXII                                  __________________________________________________________________________                      Example No.                                                                    321 322 323 324 325 326 327 328 329                           __________________________________________________________________________     Catalyst Type    FF  FF  FF  FF  FF  FF  FF  FF  FF                            Catalyst weight, gm                                                                             81.02                                                                              81.02                                                                              81.02                                                                              81.02                                                                              81.02                                                                              81.02                                                                              81.02                                                                              81.02                                                                              81.02                         Pressure, psig   598 598 598 598 598 598 600 600 600                           Temperature, °C.                                                                         258 270 259 278 269 278 279 270 270                           Time on organics, hrs.                                                                          47  52  71  76  95  99  118.5                                                                              139.8                                                                              141.5                         Duration of run, hrs.                                                                           2   2   2   2   2   2   2   1   1                             MEA SV, gmol/hr/kgcat                                                                           2.59                                                                               2.69                                                                               2.76                                                                               2.69                                                                               2.62                                                                               2.89                                                                               2.50                                                                               2.61                                                                               2.85                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              1.431                                                                              1.466                                                                              0.836                                                                              2.026                                                                              1.389                                                                              1.898                                                                              3.937                                                                              1.319                                                                              1.270                         MEA              20.803                                                                             15.928                                                                             21.573                                                                             8.455                                                                              13.153                                                                             5.684                                                                              3.430                                                                              11.218                                                                             12.033                        PIP              0.619                                                                              0.793                                                                              0.421                                                                              1.275                                                                              0.987                                                                              1.265                                                                              2.108                                                                              1.046                                                                              0.995                         DETA             41.470                                                                             40.511                                                                             47.612                                                                             36.072                                                                             40.931                                                                             31.699                                                                             26.932                                                                             37.630                                                                             37.696                        AEEA             1.655                                                                              2.044                                                                              2.654                                                                              0.991                                                                              1.869                                                                              0.695                                                                              0.297                                                                              1.784                                                                              1.787                         AEP              1.227                                                                              0.888                                                                              0.525                                                                              1.430                                                                              1.026                                                                              1.530                                                                              3.019                                                                              1.099                                                                              0.994                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             1.792                                                                              2.202                                                                              1.893                                                                              2.343                                                                              2.432                                                                              2.392                                                                              1.670                                                                              2.598                                                                              2.308                         1-TETA           9.207                                                                              11.790                                                                             9.627                                                                              13.461                                                                             13.115                                                                             13.772                                                                             11.582                                                                             14.083                                                                             12.425                        DAEP             0.616                                                                              0.258                                                                              0.103                                                                              0.671                                                                              0.399                                                                              0.778                                                                              1.863                                                                              0.456                                                                              0.383                         PEEDA            0.451                                                                              0.211                                                                              0.071                                                                              0.519                                                                              0.296                                                                              0.575                                                                              1.351                                                                              0.364                                                                              0.034                         DPE              0.029                                                                              0.076                                                                              0.066                                                                              0.203                                                                              0.107                                                                              0.217                                                                              0.107                                                                              0.049                                                                              0.059                         AE-TAEA          2.172                                                                              3.076                                                                              1.560                                                                              4.364                                                                              3.434                                                                              4.598                                                                              0.163                                                                              3.800                                                                              3.588                         1-TEPA           4.520                                                                              5.662                                                                              2.989                                                                              9.213                                                                              7.036                                                                              9.871                                                                              9.389                                                                              7.945                                                                              7.481                         AE-DAEP          0.421                                                                              0.185                                                                              0.102                                                                              0.530                                                                              0.226                                                                              6.503                                                                              0.543                                                                              0.066                                                                              0.134                         AE-PEEDA         0.029                                                                              0.036                                                                              0.030                                                                              0.116                                                                              0.035                                                                              0.100                                                                              0.907                                                                              0.030                                                                              0.098                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.023                                                                              0.000                                                                              0.000                                                                              0.223                                                                              0.050                                                                              0.264                                                                              0.161                                                                              0.068                                                                              0.138                         BPEA             0.388                                                                              0.045                                                                              0.026                                                                              0.807                                                                              0.056                                                                              1.316                                                                              1.078                                                                              0.184                                                                              0.220                         Others           3.269                                                                              3.950                                                                              1.862                                                                              7.511                                                                              4.907                                                                              4.583                                                                              16.344                                                                             5.932                                                                              7.028                         MEA Conversion, %                                                                               40.86                                                                              54.65                                                                              39.37                                                                              76.88                                                                              63.86                                                                              84.34                                                                              90.23                                                                              68.77                                                                              66.03                         DETA Conversion, %                                                                              29.93                                                                              31.45                                                                              20.47                                                                              41.38                                                                              33.16                                                                              48.10                                                                              54.39                                                                              37.75                                                                              36.75                         Acyclic(N4), %   90.94                                                                              96.25                                                                              97.95                                                                              91.90                                                                              95.09                                                                              91.15                                                                              79.97                                                                              95.05                                                                              96.87                         Acyclic(N5), %   88.61                                                                              97.05                                                                              96.63                                                                              89.01                                                                              96.62                                                                              63.88                                                                              78.03                                                                              97.13                                                                              94.95                         Σ(N5)/Σ(N4),                                                                        0.62                                                                               0.62                                                                               0.40                                                                               0.89                                                                               0.66                                                                               1.28                                                                               0.74                                                                               0.69                                                                               0.77                          weight ratio                                                                   Acyclic(N4)/cyclic                                                                              3.74                                                                               6.29                                                                               9.71                                                                               3.86                                                                               5.52                                                                               3.70                                                                               1.57                                                                               5.53                                                                               5.98                          (< = N4), weight ratio                                                         __________________________________________________________________________

                                      TABLE XXXIII                                 __________________________________________________________________________                      Example No.                                                                    330 331 332  333 334  335 336  337 338                        __________________________________________________________________________     Catalyst Type    GG  GG  GG   GG  GG   GG  GG   GG  GG                         Catalyst weight, gm                                                                             68  68  68   68  68   68  68   68  68                         Pressure, psig   606 599 602  606 593  593 601  600 600                        Temperature, °C.                                                                         270 270 280  260 270  260 280  280 270                        Time on organics, hrs.                                                                          7   26  30.5 50  55   74  79   98.8                                                                               123                        Duration of run, hrs.                                                                           2   2   1    2   2    2   2    2   2                          MEA SV, gmol/hr/kgcat                                                                           3.97                                                                               3.90                                                                               3.93 3.98                                                                               3.96 3.94                                                                               3.97 3.93                                                                               3.85                       DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00                       NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97                       Crude product composition, wt %                                                EDA              0.750                                                                              0.869                                                                              1.269                                                                               0.502                                                                              0.696                                                                               1.589                                                                              1.188                                                                               1.273                                                                              0.810                      MEA              14.139                                                                             13.058                                                                             7.841                                                                               19.884                                                                             13.962                                                                              19.078                                                                             8.661                                                                               6.995                                                                              13.582                     PIP              0.946                                                                              1.041                                                                              1.264                                                                               0.614                                                                              0.883                                                                               0.667                                                                              1.206                                                                               1.218                                                                              0.953                      DETA             42.338                                                                             40.333                                                                             34.679                                                                              47.727                                                                             41.491                                                                              46.874                                                                             37.218                                                                              33.635                                                                             40.430                     AEEA             1.641                                                                              1.480                                                                              0.679                                                                               2.213                                                                              1.609                                                                               2.241                                                                              0.609                                                                               0.617                                                                              1.541                      AEP              0.987                                                                              1.041                                                                              1.527                                                                               0.599                                                                              0.913                                                                               0.603                                                                              1.467                                                                               1.500                                                                              0.961                      HEP              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      TAEA             2.657                                                                              2.786                                                                              2.699                                                                               2.233                                                                              2.513                                                                               2.246                                                                              2.703                                                                               2.625                                                                              2.555                      1-TETA           12.825                                                                             13.469                                                                             13.932                                                                              10.488                                                                             12.891                                                                              10.468                                                                             13.856                                                                              13.911                                                                             12.446                     DAEP             0.340                                                                              0.387                                                                              0.763                                                                               0.170                                                                              0.305                                                                               0.165                                                                              0.693                                                                               0.770                                                                              0.335                      PEEDA            0.302                                                                              0.336                                                                              0.601                                                                               0.150                                                                              0.277                                                                               0.146                                                                              0.549                                                                               0.605                                                                              0.284                      DPE              0.132                                                                              0.150                                                                              0.301                                                                               0.094                                                                              0.099                                                                               0.099                                                                              0.088                                                                               0.118                                                                              0.077                      AE-TAEA          3.574                                                                              3.998                                                                              4.830                                                                               2.253                                                                              3.538                                                                               2.309                                                                              4.432                                                                               4.606                                                                              3.500                      1-TEPA           7.216                                                                              7.943                                                                              9.991                                                                               4.612                                                                              7.184                                                                               4.724                                                                              9.147                                                                               9.831                                                                              7.304                      AE-DAEP          0.088                                                                              0.082                                                                              0.204                                                                               0.154                                                                              0.134                                                                               0.064                                                                              0.601                                                                               0.879                                                                              0.328                      AE-PEEDA         0.155                                                                              0.158                                                                              0.380                                                                               0.028                                                                              0.223                                                                               0.074                                                                              0.067                                                                               0.125                                                                              0.039                      iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      AE-DPE           0.038                                                                              0.067                                                                              0.403                                                                               0.056                                                                              0.248                                                                               0.075                                                                              0.078                                                                               0.313                                                                              0.048                      BPEA             0.508                                                                              0.179                                                                              1.040                                                                               0.229                                                                              0.611                                                                               0.231                                                                              0.804                                                                               0.839                                                                              0.472                      Others           5.025                                                                              5.875                                                                              9.178                                                                               2.946                                                                              5.812                                                                               3.348                                                                              7.734                                                                               8.939                                                                              4.826                      MEA conversion, %                                                                               62.09                                                                              64.96                                                                              79.02                                                                               46.40                                                                              62.51                                                                               48.13                                                                              76.57                                                                               80.72                                                                              62.33                      DETA conversion, %                                                                              32.54                                                                              35.67                                                                              44.85                                                                               23.54                                                                              33.79                                                                               24.26                                                                              40.15                                                                               44.90                                                                              33.36                      Acyclic(N4), wt. %                                                                              95.24                                                                              94.91                                                                              90.90                                                                               96.85                                                                              95.77                                                                               96.87                                                                              92.56                                                                               91.71                                                                              95.57                      Acyclic(N5), wt. %                                                                              93.19                                                                              96.09                                                                              87.98                                                                               93.64                                                                              89.81                                                                               94.07                                                                              89.76                                                                               87.00                                                                              92.42                      Σ(N5)/Σ(N4),                                                                        0.71                                                                               0.73                                                                               0.92 0.56                                                                               0.74 0.57                                                                               0.85 0.92                                                                               0.74                       weight ratio                                                                   Acyclic(N4)/cyclic                                                                              5.72                                                                               5.50                                                                               3.73 7.82                                                                               6.22 7.57                                                                               4.14 3.93                                                                               5.75                       (< = N4), weight ratio                                                         __________________________________________________________________________                      Example No.                                                                    339 340 341 342 343 344 345 346 347 348                       __________________________________________________________________________     Catalyst Type    GG  GG  GG  GG  GG  GG  GG  GG  GG  GG                        Catalyst weight, gm                                                                             68  68  68  68  68  68  68  68  68  68                        Pressure, psig   596 598 602 603 602 602 603 603 603 603                       Temperature, °C.                                                                         271 282 260 270 260 281 272 280 272 271                       Time on organics, hrs.                                                                          158 163 182 187 206 211 272 235 254 257.5                     Duration of run, hrs.                                                                           2   2   2   2   83.7                                                                               2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           3.92                                                                               3.89                                                                               3.99                                                                               3.83                                                                               0.09                                                                               3.85                                                                               3.80                                                                               3.88                                                                               3.86                                                                               4.03                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              1.086                                                                              1.518                                                                              0.564                                                                              0.960                                                                              0.630                                                                              1.769                                                                              1.921                                                                              2.220                                                                              1.641                                                                              1.650                     MEA              13.203                                                                             6.960                                                                              18.056                                                                             12.558                                                                             17.829                                                                             6.838                                                                              12.002                                                                             5.827                                                                              11.663                                                                             13.072                    PIP              1.186                                                                              1.446                                                                              0.765                                                                              1.101                                                                              0.770                                                                              1.362                                                                              1.263                                                                              1.380                                                                              1.178                                                                              1.205                     DETA             40.181                                                                             35.494                                                                             45.781                                                                             40.874                                                                             44.267                                                                             34.368                                                                             39.115                                                                             30.652                                                                             38.907                                                                             40.441                    AEEA             1.261                                                                              0.505                                                                              2.117                                                                              1.385                                                                              2.108                                                                              0.517                                                                              1.158                                                                              0.441                                                                              1.197                                                                              1.308                     AEP              1.136                                                                              1.798                                                                              0.738                                                                              1.161                                                                              0.699                                                                              1.725                                                                              1.205                                                                              1.595                                                                              1.179                                                                              1.119                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             2.661                                                                              2.671                                                                              2.384                                                                              2.732                                                                              2.320                                                                              2.531                                                                              2.548                                                                              2.402                                                                              2.575                                                                              2.513                     1-TETA           13.232                                                                             14.206                                                                             11.386                                                                             13.549                                                                             11.117                                                                             13.437                                                                             12.752                                                                             13.162                                                                             12.893                                                                             12.524                    DAEP             0.452                                                                              0.939                                                                              0.225                                                                              0.438                                                                              0.196                                                                              0.889                                                                              0.485                                                                              0.981                                                                              0.469                                                                              0.410                     PEEDA            0.372                                                                              0.692                                                                              0.187                                                                              0.361                                                                              0.175                                                                              0.670                                                                              0.383                                                                              0.728                                                                              0.375                                                                              0.335                     DPE              0.076                                                                              0.107                                                                              0.056                                                                              0.091                                                                              0.033                                                                              0.111                                                                              0.077                                                                              0.133                                                                              0.082                                                                              0.076                     AE-TAEA          4.013                                                                              4.667                                                                              2.669                                                                              3.990                                                                              2.705                                                                              4.603                                                                              4.023                                                                              4.890                                                                              3.878                                                                              3.770                     1-TEPA           8.152                                                                              9.680                                                                              5.588                                                                              8.225                                                                              5.696                                                                              9.840                                                                              8.145                                                                              10.433                                                                             8.054                                                                              7.706                     AE-DAEP          0.401                                                                              0.783                                                                              0.156                                                                              0.382                                                                              0.201                                                                              0.171                                                                              0.377                                                                              0.235                                                                              0.379                                                                              0.324                     AE-PEEDA         0.047                                                                              0.080                                                                              0.028                                                                              0.051                                                                              0.028                                                                              0.114                                                                              0.042                                                                              0.161                                                                              0.048                                                                              0.037                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.057                                                                              0.105                                                                              0.046                                                                              0.043                                                                              0.036                                                                              0.053                                                                              0.049                                                                              0.706                                                                              0.047                                                                              0.046                     BPEA             0.607                                                                              0.902                                                                              0.324                                                                              0.630                                                                              0.311                                                                              0.897                                                                              0.644                                                                              1.020                                                                              0.619                                                                              0.582                     Others           5.537                                                                              8.116                                                                              3.310                                                                              5.711                                                                              3.339                                                                              10.005                                                                             5.502                                                                              13.484                                                                             5.564                                                                              5.184                     MEA conversion, %                                                                               64.77                                                                              81.20                                                                              51.33                                                                              66.74                                                                              50.94                                                                              81.35                                                                              67.32                                                                              84.30                                                                              67.93                                                                              64.52                     DETA conversion, %                                                                              36.28                                                                              43.03                                                                              26.65                                                                              35.67                                                                              27.60                                                                              44.30                                                                              36.70                                                                              50.93                                                                              36.43                                                                              34.77                     Acyclic(N4), wt. %                                                                              94.64                                                                              90.67                                                                              96.72                                                                              94.81                                                                              97.08                                                                              90.53                                                                              94.19                                                                              89.41                                                                              94.35                                                                              94.83                     Acyclic(N5), wt. %                                                                              91.63                                                                              88.47                                                                              93.71                                                                              91.70                                                                              93.58                                                                              92.12                                                                              91.63                                                                              87.84                                                                              91.61                                                                              92.07                     Σ(N5)/Σ(N4), weight ratio                                                           0.79                                                                               0.87                                                                               0.62                                                                               0.78                                                                               0.65                                                                               0.89                                                                               0.82                                                                               1.00                                                                               0.79                                                                               0.79                      Acyclic(N4)/cyclic(< = N4),                                                                     4.93                                                                               3.39                                                                               6.99                                                                               5.16                                                                               7.17                                                                               3.36                                                                               4.48                                                                               3.23                                                                               4.71                                                                               4.78                      weight ratio                                                                   __________________________________________________________________________                      Example No.                                                                    349 350 351  352 353  354 355  356 357                        __________________________________________________________________________     Catalyst Type    GG  GG  GG   GG  GG   GG  GG   GG  GG                         Catalyst weight, gm                                                                             67.2                                                                               67.2                                                                               67.2 67.2                                                                               67.2 67.2                                                                               67.2 67.2                                                                               67.2                       Pressure, psig   600 600 600  600 600  600 600  600 600                        Temperature, °C.                                                                         267.7                                                                              267.9                                                                              278  257.8                                                                              269.6                                                                               259.3                                                                              279.3                                                                               269.8                                                                              270.1                      Time on organics, hrs.                                                                          4   6.5 28.5 47.5                                                                               52.5 71  76.5 96.5                                                                               99                         Duration of run, hrs.                                                                           2   2   2    2   2    2   2    2   2                          MEA SV, gmol/hr/kgcat                                                                           4.59                                                                               4.81                                                                               4.66 4.74                                                                               4.80 4.79                                                                               4.46 4.63                                                                               4.60                       DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00                       NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97                       Crude product composition, wt. %                                               EDA              0.515                                                                              0.541                                                                              1.593                                                                               0.567                                                                              0.832                                                                               0.445                                                                              1.675                                                                               0.932                                                                              0.995                      MEA              23.588                                                                             25.727                                                                             18.012                                                                              26.580                                                                             21.992                                                                              27.189                                                                             13.854                                                                              20.859                                                                             20.291                     PIP              0.888                                                                              1.118                                                                              1.953                                                                               1.009                                                                              1.390                                                                               0.957                                                                              1.810                                                                               1.493                                                                              1.486                      DETA             54.811                                                                             54.100                                                                             50.845                                                                              55.433                                                                             53.042                                                                              56.685                                                                             51.796                                                                              53.039                                                                             51.623                     AEEA             0.344                                                                              0.802                                                                              0.233                                                                               0.360                                                                              0.208                                                                               0.377                                                                              0.150                                                                               0.478                                                                              0.210                      AEP              0.883                                                                              0.858                                                                              1.884                                                                               0.856                                                                              1.352                                                                               0.775                                                                              2.177                                                                               1.423                                                                              1.423                      HEP              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      TAEA             1.618                                                                              1.490                                                                              1.878                                                                               1.474                                                                              1.695                                                                               1.397                                                                              1.977                                                                               1.858                                                                              1.955                      1-TETA           7.964                                                                              7.269                                                                              9.198                                                                               6.586                                                                              8.327                                                                               6.490                                                                              9.962                                                                               8.880                                                                              10.270                     DAEP             0.114                                                                              0.093                                                                              0.645                                                                               0.301                                                                              0.154                                                                               0.207                                                                              0.692                                                                               0.412                                                                              0.178                      PEEDA            0.081                                                                              0.064                                                                              0.387                                                                               0.144                                                                              0.104                                                                               0.117                                                                              0.359                                                                               0.162                                                                              0.125                      DPE              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      AE-TAEA          0.000                                                                              0.088                                                                              0.246                                                                               0.000                                                                              0.102                                                                               0.000                                                                              1.894                                                                               0.109                                                                              0.000                      1-TEPA           0.664                                                                              0.704                                                                              1.555                                                                               0.500                                                                              0.975                                                                               0.246                                                                              3.556                                                                               1.157                                                                              1.321                      AE-DAEP          0.000                                                                              0.223                                                                              0.372                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.114                                                                               0.133                                                                              0.326                      AE-PEEDA         0.000                                                                              0.000                                                                              0.099                                                                               0.000                                                                              0.175                                                                               0.000                                                                              0.075                                                                               0.000                                                                              0.069                      iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      AE-DPE           0.168                                                                              0.000                                                                              0.059                                                                               0.000                                                                              0.423                                                                               0.000                                                                              0.000                                                                               0.083                                                                              0.512                      BPEA             0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      Others           1.532                                                                              0.963                                                                              2.990                                                                               1.492                                                                              2.047                                                                               0.994                                                                              0.880                                                                               1.861                                                                              2.579                      MEA conversion, %                                                                               34.18                                                                              28.60                                                                              49.97                                                                               27.10                                                                              38.81                                                                               25.75                                                                              61.46                                                                               42.13                                                                              44.20                      DETA conversion, %                                                                              9.11                                                                               10.77                                                                              16.06                                                                               9.64                                                                               12.29                                                                               7.99                                                                               14.37                                                                               12.55                                                                              15.64                      Acyclic(N4), wt. %                                                                              98.01                                                                              98.23                                                                              91.48                                                                               94.77                                                                              97.49                                                                               96.05                                                                              91.91                                                                               94.93                                                                              97.59                      Acyclic(N5), wt. %                                                                              79.79                                                                              78.07                                                                              77.26                                                                               100.00                                                                             64.30                                                                               100.00                                                                             96.64                                                                               85.40                                                                              59.30                      Σ(N5)/Σ(N4), weight ratio                                                           0.09                                                                               0.11                                                                               0.19 0.06                                                                               0.16 0.03                                                                               0.43 0.13                                                                               0.18                       Acyclic(N4)/cyclic(< = N4),                                                                     4.87                                                                               4.11                                                                               2.27 3.49                                                                               3.34 3.83                                                                               2.37 3.08                                                                               3.81                       weight ratio                                                                   __________________________________________________________________________

                                      TABLE XXXIV                                  __________________________________________________________________________                      Example No.                                                                    358 359 360  361 362  363 364  365 366                        __________________________________________________________________________     Catalyst Type    HH  HH  HH   HH  HH   HH  HH   HH  HH                         Catalyst weight, gm                                                                             69.34                                                                              69.34                                                                              69.34                                                                               69.34                                                                              69.34                                                                               69.34                                                                              69.34                                                                               69.34                                                                              69.34                      Pressure, psig   604 603 603  604 604  603 603  600 600                        Temperature, °C.                                                                         270 270 280  260 270  260 280  280 270                        Time on organics, hrs.                                                                          7   26  30.5 50  55   74  79   98.8                                                                               123                        Duration of run, hrs.                                                                           2   2   1    2   2    2   2    2   2                          MEA SV, gmol/hr/kgcat                                                                           4.33                                                                               4.26                                                                               4.21 4.20                                                                               4.33 4.20                                                                               4.17 4.26                                                                               4.16                       DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00                       NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97                       Crude product composition, wt. %                                               EDA              0.805                                                                              1.034                                                                              1.662                                                                               0.510                                                                              0.908                                                                               0.544                                                                              1.363                                                                               2.077                                                                              0.963                      MEA              14.316                                                                             13.747                                                                             10.093                                                                              20.646                                                                             15.418                                                                              19.410                                                                             8.991                                                                               9.550                                                                              15.047                     PIP              0.832                                                                              0.927                                                                              1.260                                                                               0.542                                                                              0.841                                                                               0.555                                                                              1.085                                                                               1.325                                                                              0.906                      DETA             41.647                                                                             40.641                                                                             36.709                                                                              48.819                                                                             43.537                                                                              47.902                                                                             35.150                                                                              32.997                                                                             41.105                     AEEA             1.392                                                                              1.332                                                                              0.661                                                                               2.056                                                                              1.526                                                                               2.142                                                                              0.718                                                                               0.580                                                                              1.445                      AEP              0.990                                                                              1.057                                                                              1.455                                                                               0.554                                                                              0.915                                                                               0.588                                                                              1.336                                                                               1.810                                                                              0.927                      HEP              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      TAEA             2.980                                                                              2.906                                                                              2.683                                                                               2.272                                                                              2.709                                                                               2.329                                                                              2.593                                                                               1.994                                                                              2.443                      1-TETA           13.276                                                                             13.074                                                                             12.859                                                                              9.750                                                                              12.028                                                                              10.013                                                                             12.850                                                                              10.946                                                                             11.547                     DAEP             0.416                                                                              0.470                                                                              0.726                                                                               0.152                                                                              0.358                                                                               0.171                                                                              0.754                                                                               1.270                                                                              0.373                      PEEDA            0.321                                                                              0.347                                                                              0.527                                                                               0.130                                                                              0.270                                                                               0.147                                                                              0.531                                                                               0.858                                                                              0.292                      DPE              0.151                                                                              0.167                                                                              0.208                                                                               0.055                                                                              0.159                                                                               0.073                                                                              0.126                                                                               0.164                                                                              0.196                      AE-TAEA          4.148                                                                              4.074                                                                              4.997                                                                               2.219                                                                              3.441                                                                               2.254                                                                              4.357                                                                               3.447                                                                              3.193                      1-TEPA           7.057                                                                              7.074                                                                              8.378                                                                               3.718                                                                              6.209                                                                               3.871                                                                              8.283                                                                               7.231                                                                              6.092                      AE-DAEP          0.081                                                                              0.074                                                                              0.124                                                                               0.145                                                                              0.075                                                                               0.247                                                                              1.053                                                                               1.912                                                                              0.489                      AE-PEEDA         0.148                                                                              0.141                                                                              0.238                                                                               0.027                                                                              0.117                                                                               0.067                                                                              0.154                                                                               0.294                                                                              0.065                      iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      AE-DPE           0.051                                                                              0.069                                                                              0.286                                                                               0.266                                                                              0.175                                                                               0.261                                                                              0.309                                                                               0.130                                                                              0.070                      BPEA             0.582                                                                              0.570                                                                              0.800                                                                               0.207                                                                              0.479                                                                               0.205                                                                              0.737                                                                               0.613                                                                              0.415                      Others           5.099                                                                              5.415                                                                              7.215                                                                               2.423                                                                              4.615                                                                               2.781                                                                              8.931                                                                               12.620                                                                             4.609                      MEA conversion, %                                                                               61.90                                                                              63.00                                                                              72.52                                                                               43.91                                                                              58.54                                                                               46.90                                                                              75.19                                                                               73.83                                                                              57.94                      DETA conversion, %                                                                              34.13                                                                              35.00                                                                              40.60                                                                               21.18                                                                              30.42                                                                               22.12                                                                              42.36                                                                               46.26                                                                              31.71                      Acyclic(N4), wt. %                                                                              94.82                                                                              94.20                                                                              91.41                                                                               97.28                                                                              94.93                                                                               96.93                                                                              91.63                                                                               84.95                                                                              94.20                      Acyclic(N5), wt. %                                                                              92.86                                                                              92.88                                                                              90.23                                                                               90.21                                                                              91.94                                                                               88.71                                                                              84.88                                                                               78.36                                                                              89.93                      Σ(N5)/Σ(N4), weight ratio                                                           0.70                                                                               0.71                                                                               0.87 0.53                                                                               0.68 0.54                                                                               0.88 0.89                                                                               0.70                       Acyclic(N4)/cyclic(< = N4),                                                                     6.00                                                                               5.38                                                                               3.72 8.39                                                                               5.80 8.05                                                                               4.03 2.38                                                                               5.19                       weight ratio                                                                   __________________________________________________________________________                      Example No.                                                                    367 368 369 370 371 372 373 374 375 376                       __________________________________________________________________________     Catalyst Type    HH  HH  HH  HH  HH  HH  HH  HH  HH  HH                        Catalyst weight, gm                                                                             69.34                                                                              69.34                                                                              69.34                                                                              69.34                                                                              69.34                                                                              69.34                                                                              69.34                                                                              69.34                                                                              69.34                                                                              69.34                     Pressure, psig   603 604 603 604 603 604 604 604 603 604                       Temperature, °C.                                                                         271 282 260 270 260 281 272 280 272 271                       Time on organics, hrs.                                                                          158 163 182 187 206 211 272 235 254 257.5                     Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           4.01                                                                               4.31                                                                               4.28                                                                               4.05                                                                               4.11                                                                               4.41                                                                               4.13                                                                               4.11                                                                               4.22                                                                               4.43                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              1.212                                                                              1.778                                                                              0.757                                                                              0.980                                                                              0.861                                                                              2.156                                                                              1.946                                                                              2.350                                                                              1.794                                                                              1.594                     MEA              12.554                                                                             9.298                                                                              20.034                                                                             13.105                                                                             18.882                                                                             8.720                                                                              12.941                                                                             7.170                                                                              13.118                                                                             13.362                    PIP              1.009                                                                              1.387                                                                              0.734                                                                              0.962                                                                              0.794                                                                              1.385                                                                              1.150                                                                              1.343                                                                              1.147                                                                              1.045                     DETA             37.117                                                                             36.552                                                                             46.016                                                                             38.892                                                                             44.565                                                                             34.824                                                                             39.610                                                                             33.663                                                                             39.912                                                                             38.851                    AEEA             1.046                                                                              0.554                                                                              1.888                                                                              1.280                                                                              1.745                                                                              0.521                                                                              1.185                                                                              0.478                                                                              1.195                                                                              1.279                     AEP              1.212                                                                              1.598                                                                              0.679                                                                              0.976                                                                              0.784                                                                              1.518                                                                              1.109                                                                              1.669                                                                              1.094                                                                              1.015                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             2.311                                                                              2.549                                                                              2.223                                                                              2.513                                                                              2.187                                                                              2.296                                                                              2.546                                                                              2.452                                                                              2.458                                                                              2.496                     1-TETA           11.703                                                                             13.076                                                                             10.211                                                                             11.973                                                                             10.178                                                                             12.160                                                                             12.466                                                                             13.106                                                                             12.081                                                                             12.149                    DAEP             0.669                                                                              0.839                                                                              0.209                                                                              0.394                                                                              0.335                                                                              0.916                                                                              0.518                                                                              1.012                                                                              0.454                                                                              0.423                     PEEDA            0.476                                                                              0.594                                                                              0.174                                                                              0.318                                                                              0.240                                                                              0.634                                                                              0.377                                                                              0.766                                                                              0.348                                                                              0.321                     DPE              0.112                                                                              0.468                                                                              0.072                                                                              0.186                                                                              0.150                                                                              0.127                                                                              0.092                                                                              0.123                                                                              0.079                                                                              0.072                     AE-TAEA          3.397                                                                              4.484                                                                              2.580                                                                              3.922                                                                              2.727                                                                              4.290                                                                              3.863                                                                              4.417                                                                              3.624                                                                              3.540                     1-TEPA           7.003                                                                              8.450                                                                              5.015                                                                              7.390                                                                              5.407                                                                              8.840                                                                              7.583                                                                              9.218                                                                              7.097                                                                              6.990                     AE-DAEP          0.928                                                                              0.694                                                                              0.198                                                                              0.427                                                                              0.351                                                                              0.189                                                                              0.411                                                                              0.892                                                                              0.342                                                                              0.038                     AE-PEEDA         0.153                                                                              0.085                                                                              0.045                                                                              0.079                                                                              0.059                                                                              0.132                                                                              0.052                                                                              0.135                                                                              0.036                                                                              0.038                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.287                                                                              0.093                                                                              0.051                                                                              0.166                                                                              0.042                                                                              0.411                                                                              0.073                                                                              0.390                                                                              0.091                                                                              0.061                     BPEA             0.510                                                                              0.761                                                                              0.054                                                                              0.563                                                                              0.330                                                                              0.822                                                                              0.597                                                                              0.843                                                                              0.577                                                                              0.535                     Others           7.302                                                                              7.358                                                                              3.390                                                                              6.493                                                                              3.912                                                                              10.339                                                                             5.881                                                                              9.704                                                                              5.473                                                                              5.321                     Conversion, %    64.82                                                                              74.69                                                                              45.65                                                                              63.83                                                                              48.59                                                                              76.20                                                                              64.94                                                                              80.41                                                                              63.82                                                                              62.91                     DETA conversion, %                                                                              38.19                                                                              40.86                                                                              25.81                                                                              36.20                                                                              27.88                                                                              43.50                                                                              36.22                                                                              45.35                                                                              34.58                                                                              34.25                     Acyclic(N4), wt. %                                                                              91.77                                                                              89.15                                                                              96.47                                                                              94.16                                                                              94.46                                                                              89.61                                                                              93.83                                                                              89.12                                                                              94.28                                                                              94.72                     Acyclic(N5), wt. %                                                                              84.70                                                                              88.79                                                                              95.62                                                                              90.16                                                                              91.23                                                                              89.42                                                                              91.00                                                                              85.78                                                                              91.11                                                                              91.63                     Σ(N5)/Σ(N4), weight ratio                                                           0.80                                                                               0.83                                                                               0.62                                                                               0.82                                                                               0.68                                                                               0.91                                                                               0.79                                                                               0.91                                                                               0.76                                                                               0.74                      Acyclic(N4)/cyclic(< = N4),                                                                     4.03                                                                               3.20                                                                               6.65                                                                               5.11                                                                               5.37                                                                               3.16                                                                               4.63                                                                               3.17                                                                               4.66                                                                               5.09                      weight ratio                                                                   __________________________________________________________________________

                                      TABLE XXXV                                   __________________________________________________________________________                      Example No.                                                                    377 378 379 380 381 382 383 384 385                           __________________________________________________________________________     Catalyst Type    II  II  II  II  II  II  II  II  II                            Catalyst weight, gm                                                                             70.6                                                                               70.6                                                                               70.6                                                                               70.6                                                                               70.6                                                                               70.6                                                                               70.6                                                                               70.6                                                                               70.6                          Pressure, psig   600 600 600 600 600 600 600 600 600                           Temperature, °C.                                                                         267.7                                                                              267.9                                                                              278 257.8                                                                              269.6                                                                              259.3                                                                              279.3                                                                              269.8                                                                              270.1                         Time on organics, hrs.                                                                          4   6.5 30.5                                                                               49.5                                                                               54.5                                                                               73  78.5                                                                               98  101                           Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2                             MEA SV, gmol/hr/kgcat                                                                           4.23                                                                               4.29                                                                               4.10                                                                               4.04                                                                               4.14                                                                               4.15                                                                               3.89                                                                               3.94                                                                               3.95                          DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                          NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                          Crude product composition, wt. %                                               EDA              0.162                                                                              0.169                                                                              0.783                                                                              0.192                                                                              0.397                                                                              0.176                                                                              1.073                                                                              0.529                                                                              0.553                         MEA              29.144                                                                             31.908                                                                             24.483                                                                             32.053                                                                             27.952                                                                             31.487                                                                             22.456                                                                             25.861                                                                             26.009                        PIP              0.349                                                                              0.340                                                                              1.209                                                                              0.251                                                                              0.651                                                                              0.248                                                                              1.406                                                                              0.768                                                                              0.760                         DETA             59.742                                                                             58.534                                                                             56.565                                                                             58.955                                                                             59.279                                                                             59.506                                                                             54.811                                                                             57.648                                                                             57.364                        AEEA             0.310                                                                              0.929                                                                              0.200                                                                              0.321                                                                              0.342                                                                              0.351                                                                              0.776                                                                              0.366                                                                              0.370                         AEP              0.544                                                                              0.498                                                                              1.287                                                                              0.436                                                                              0.711                                                                              0.471                                                                              1.454                                                                              0.793                                                                              0.801                         HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         TAEA             0.578                                                                              0.706                                                                              0.873                                                                              0.618                                                                              0.733                                                                              0.669                                                                              1.573                                                                              0.874                                                                              1.310                         1-TETA           4.153                                                                              2.968                                                                              6.200                                                                              2.623                                                                              4.926                                                                              2.835                                                                              6.907                                                                              5.628                                                                              5.841                         DAEP             0.177                                                                              0.175                                                                              0.342                                                                              0.144                                                                              0.238                                                                              0.180                                                                              0.520                                                                              0.239                                                                              0.184                         PEEDA            0.076                                                                              0.000                                                                              0.220                                                                              0.000                                                                              0.135                                                                              0.000                                                                              0.347                                                                              0.085                                                                              0.125                         DPE              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.060                                                                              0.000                                                                              0.000                         AE-TAEA          0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.236                                                                              0.000                                                                              0.000                         1-TEPA           0.000                                                                              0.000                                                                              0.463                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.848                                                                              0.318                                                                              0.401                         AE-DAEP          0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.181                                                                              0.000                                                                              0.000                         AE-PEEDA         0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         AE-DPE           0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.279                                                                              0.000                                                                              0.000                         BPEA             0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                         Others           0.976                                                                              0.215                                                                              1.483                                                                              1.078                                                                              1.416                                                                              1.247                                                                              1.734                                                                              1.491                                                                              2.212                         MEA conversion, %                                                                               20.13                                                                              12.23                                                                              32.26                                                                              12.02                                                                              24.15                                                                              14.16                                                                              38.70                                                                              28.47                                                                              29.14                         DETA conversion, %                                                                              2.69                                                                               4.31                                                                               6.99                                                                               3.83                                                                               4.40                                                                               3.59                                                                               11.07                                                                              5.24                                                                               7.12                          Acyclic(N4), wt. %                                                                              94.94                                                                              95.46                                                                              92.64                                                                              95.76                                                                              93.82                                                                              95.11                                                                              90.14                                                                              95.25                                                                              95.85                         Acyclic(N5), wt. %                                                                              --  --  100.00                                                                             --  --  --  70.20                                                                              100.00                                                                             100.00                        Σ(N5)/Σ(N4), weight ratio                                                           0.00                                                                               0.00                                                                               0.00                                                                               0.00                                                                               0.00                                                                               0.00                                                                               0.16                                                                               0.05                                                                               0.05                          Acyclic(N4)/cyclic(< = N4),                                                                     4.13                                                                               3.63                                                                               2.31                                                                               3.90                                                                               3.26                                                                               3.90                                                                               2.24                                                                               3.45                                                                               3.82                          weight ratio                                                                   __________________________________________________________________________

                                      TABLE XXXVI                                  __________________________________________________________________________                      Example No.                                                                    386 387 388  389 390  391 392  393 394                        __________________________________________________________________________     Catalyst Type    JJ  JJ  JJ   JJ  JJ   JJ  JJ   JJ  JJ                         Catalyst weight, gm                                                                             67.5                                                                               67.5                                                                               67.5 67.5                                                                               67.5 67.5                                                                               67.5 67.5                                                                               67.5                       Pressure, psig   598 597 597  598 598  598 598  600 600                        Temperature, °C.                                                                         270 270 280  260 270  260 280  280 270                        Time on organics, hrs.                                                                          7   26  30.5 50  55   74  79   98.8                                                                               123                        Duration of run, hrs.                                                                           2   2   1    2   2    2   2    2   2                          MEA SV, gmol/hr/kgcat                                                                           3.62                                                                               3.73                                                                               3.53 3.46                                                                               3.70 3.56                                                                               3.47 3.46                                                                               3.40                       DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00 1.00                                                                               1.00                       NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97 5.97                                                                               5.97                       Crude product composition, wt. %                                               EDA              0.294                                                                              0.424                                                                              0.706                                                                               0.273                                                                              0.506                                                                               0.342                                                                              0.979                                                                               1.001                                                                              0.624                      MEA              25.314                                                                             22.475                                                                             18.589                                                                              26.092                                                                             22.747                                                                              25.743                                                                             18.317                                                                              16.142                                                                             21.635                     PIP              0.421                                                                              0.496                                                                              0.707                                                                               0.266                                                                              0.485                                                                               0.297                                                                              0.712                                                                               0.692                                                                              0.469                      DETA             54.036                                                                             51.203                                                                             48.723                                                                              54.115                                                                             52.329                                                                              54.167                                                                             48.580                                                                              42.653                                                                             47.745                     AEEA             1.899                                                                              2.033                                                                              1.670                                                                               2.115                                                                              2.193                                                                               2.258                                                                              1.799                                                                               1.403                                                                              1.963                      AEP              0.488                                                                              0.616                                                                              0.869                                                                               0.374                                                                              0.614                                                                               0.438                                                                              0.855                                                                               0.848                                                                              0.588                      HEP              0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      TAEA             1.340                                                                              1.728                                                                              1.888                                                                               1.215                                                                              1.590                                                                               1.290                                                                              1.768                                                                               1.764                                                                              1.551                      1-TETA           6.203                                                                              8.239                                                                              9.101                                                                               5.680                                                                              7.515                                                                               6.023                                                                              8.740                                                                               9.202                                                                              7.737                      DAEP             0.091                                                                              0.205                                                                              0.282                                                                               0.096                                                                              0.157                                                                               0.110                                                                              0.267                                                                               0.415                                                                              0.216                      PEEDA            0.093                                                                              0.162                                                                              0.229                                                                               0.076                                                                              0.133                                                                               0.090                                                                              0.209                                                                               0.313                                                                              0.172                      DPE              0.048                                                                              0.111                                                                              0.178                                                                               0.076                                                                              0.126                                                                               0.084                                                                              0.220                                                                               0.387                                                                              0.232                      AE-TAEA          1.230                                                                              1.884                                                                              2.347                                                                               1.338                                                                              1.704                                                                               1.006                                                                              1.902                                                                               2.806                                                                              1.832                      1-TEPA           2.363                                                                              3.385                                                                              4.197                                                                               1.841                                                                              2.798                                                                               1.882                                                                              3.504                                                                               5.099                                                                              3.159                      AE-DAEP          0.139                                                                              0.145                                                                              0.257                                                                               0.143                                                                              0.273                                                                               0.114                                                                              0.392                                                                               0.812                                                                              0.539                      AE-PEEDA         0.066                                                                              0.034                                                                              0.101                                                                               0.042                                                                              0.061                                                                               0.024                                                                              0.100                                                                               0.168                                                                              0.078                      iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                                                                               0.000                                                                              0.000                      AE-DPE           0.000                                                                              0.043                                                                              0.117                                                                               0.077                                                                              0.157                                                                               0.090                                                                              0.062                                                                               0.343                                                                              0.035                      BPEA             0.110                                                                              0.211                                                                              0.290                                                                               0.056                                                                              0.110                                                                               0.069                                                                              0.063                                                                               0.209                                                                              0.048                      Others           2.415                                                                              3.286                                                                              4.610                                                                               2.509                                                                              3.660                                                                               2.432                                                                              4.633                                                                               8.202                                                                              4.835                      MEA conversion, %                                                                               31.77                                                                              40.08                                                                              50.03                                                                               29.37                                                                              39.57                                                                               30.42                                                                              49.72                                                                               55.92                                                                              40.42                      DETA conversion, %                                                                              13.44                                                                              18.87                                                                              22.15                                                                               12.94                                                                              17.39                                                                               12.99                                                                              20.75                                                                               30.77                                                                              21.85                      Acyclic(N4), wt. %                                                                              97.01                                                                              95.43                                                                              94.10                                                                               96.54                                                                              95.63                                                                               96.27                                                                              93.80                                                                               90.77                                                                              93.73                      Acyclic(N5), wt. %                                                                              91.93                                                                              92.41                                                                              89.53                                                                               90.91                                                                              88.22                                                                               90.67                                                                              89.75                                                                               83.77                                                                              87.68                      Σ(N5)/Σ(N4), weight ratio                                                           0.50                                                                               0.55                                                                               0.63 0.49                                                                               0.54 0.42                                                                               0.54 0.78                                                                               0.57                       Acyclic(N4)/cyclic(< = N4),                                                                     6.61                                                                               6.27                                                                               4.85 7.78                                                                               6.01 7.18                                                                               4.65 4.13                                                                               5.53                       weight ratio                                                                   __________________________________________________________________________                      Example No.                                                                    395 396 397 398 399 400 401 402 403 404                       __________________________________________________________________________     Catalyst Type    JJ  JJ  JJ  JJ  JJ  JJ  JJ  JJ  JJ  JJ                        Catalyst weight, gm                                                                             67.5                                                                               67.5                                                                               67.5                                                                               67.5                                                                               67.5                                                                               67.5                                                                               67.5                                                                               67.5                                                                               67.5                                                                               67.5                      Pressure, psig   585 598 598 598 598 598 598 598 598 598                       Temperature, °C.                                                                         271 282 260 270 260 281 272 280 272 271                       Time on organics, hrs.                                                                          158 163 182 187 206 211 272 235 254 257.5                     Duration of run, hrs.                                                                           2   2   2   2   2   2   2   2   2   2                         MEA SV, gmol/hr/kgcat                                                                           2.97                                                                               3.69                                                                               3.58                                                                               3.41                                                                               3.41                                                                               3.54                                                                               3.99                                                                               3.53                                                                               3.50                                                                               3.70                      DETA/MEA mole ratio                                                                             1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                                                                               1.00                      NH.sub.3 /MEA mole ratio                                                                        5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                                                                               5.97                      Crude product composition, wt. %                                               EDA              0.764                                                                              1.129                                                                              0.479                                                                              0.786                                                                              0.509                                                                              1.756                                                                              1.803                                                                              1.993                                                                              1.749                                                                              1.597                     MEA              20.571                                                                             16.885                                                                             25.262                                                                             21.504                                                                             25.342                                                                             18.397                                                                             20.631                                                                             15.100                                                                             20.996                                                                             22.350                    PIP              0.531                                                                              0.826                                                                              0.351                                                                              0.538                                                                              0.352                                                                              0.865                                                                              0.634                                                                              0.781                                                                              0.638                                                                              0.567                     DETA             47.941                                                                             46.768                                                                             52.656                                                                             48.687                                                                             51.138                                                                             47.357                                                                             46.647                                                                             42.162                                                                             46.440                                                                             48.370                    AEEA             1.707                                                                              1.530                                                                              2.132                                                                              1.979                                                                              2.129                                                                              1.620                                                                              1.738                                                                              1.446                                                                              1.730                                                                              1.824                     AEP              0.697                                                                              1.034                                                                              0.470                                                                              0.636                                                                              0.432                                                                              0.927                                                                              0.707                                                                              0.935                                                                              0.676                                                                              0.626                     HEP              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     TAEA             1.641                                                                              1.964                                                                              1.408                                                                              1.541                                                                              1.337                                                                              1.743                                                                              1.648                                                                              1.942                                                                              1.596                                                                              1.530                     1-TETA           8.006                                                                              9.717                                                                              6.641                                                                              7.305                                                                              6.278                                                                              8.432                                                                              8.037                                                                              9.595                                                                              7.922                                                                              7.422                     DAEP             0.239                                                                              0.408                                                                              0.135                                                                              0.174                                                                              0.125                                                                              0.291                                                                              0.359                                                                              0.442                                                                              0.295                                                                              0.232                     PEEDA            0.186                                                                              0.297                                                                              0.101                                                                              0.138                                                                              0.094                                                                              0.224                                                                              0.234                                                                              0.314                                                                              0.215                                                                              0.169                     DPE              0.211                                                                              0.069                                                                              0.110                                                                              0.183                                                                              0.114                                                                              0.089                                                                              0.099                                                                              0.103                                                                              0.182                                                                              0.107                     AE-TAEA          1.858                                                                              2.661                                                                              1.266                                                                              1.659                                                                              1.462                                                                              2.013                                                                              2.165                                                                              2.975                                                                              2.063                                                                              1.905                     1-TEPA           3.247                                                                              5.154                                                                              2.314                                                                              2.935                                                                              2.396                                                                              3.688                                                                              3.984                                                                              5.395                                                                              3.860                                                                              3.394                     AE-DAEP          0.401                                                                              0.342                                                                              0.130                                                                              0.223                                                                              0.173                                                                              0.261                                                                              0.335                                                                              0.507                                                                              0.256                                                                              0.234                     AE-PEEDA         0.057                                                                              0.062                                                                              0.025                                                                              0.068                                                                              0.063                                                                              0.045                                                                              0.076                                                                              0.117                                                                              0.056                                                                              0.042                     iAE-PEEDA        0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                                                                              0.000                     AE-DPE           0.053                                                                              0.067                                                                              0.086                                                                              0.211                                                                              0.083                                                                              0.034                                                                              0.229                                                                              0.080                                                                              0.055                                                                              0.040                     BPEA             0.051                                                                              0.390                                                                              0.040                                                                              0.087                                                                              0.037                                                                              0.225                                                                              0.294                                                                              0.465                                                                              0.272                                                                              0.231                     Others           4.459                                                                              5.997                                                                              2.874                                                                              5.176                                                                              3.565                                                                              5.035                                                                              6.180                                                                              8.307                                                                              5.107                                                                              4.381                     MEA conversion, %                                                                               42.93                                                                              55.07                                                                              31.89                                                                              40.98                                                                              31.07                                                                              49.41                                                                              44.79                                                                              58.84                                                                              42.66                                                                              39.29                     DETA conversion, %                                                                              20.95                                                                              26.04                                                                              15.63                                                                              20.58                                                                              17.33                                                                              22.60                                                                              25.81                                                                              31.71                                                                              24.63                                                                              31.91                     Acyclic(N4), wt. %                                                                              93.81                                                                              93.79                                                                              95.88                                                                              94.70                                                                              95.80                                                                              94.40                                                                              93.33                                                                              93.06                                                                              93.21                                                                              94.64                     Acyclic(N5), wt. %                                                                              90.08                                                                              90.08                                                                              92.72                                                                              88.64                                                                              91.56                                                                              90.98                                                                              86.82                                                                              87.74                                                                              90.25                                                                              90.67                     Σ(N5)/Σ(N4), weight ratio                                                           0.55                                                                               0.70                                                                               0.46                                                                               0.55                                                                               0.53                                                                               0.58                                                                               0.68                                                                               0.77                                                                               0.64                                                                               0.62                      Acyclic(N4)/cyclic(< = N4),                                                                     5.17                                                                               4.43                                                                               6.90                                                                               5.30                                                                               6.82                                                                               4.25                                                                               4.76                                                                               4.48                                                                               4.74                                                                               5.26                      weight ratio                                                                   __________________________________________________________________________

Although the invention has been illustrated by certain of the preceding examples, it is not to be construed as being limited thereby; but rather, the invention encompasses the generic area as hereinbefore disclosed. Various modifications and embodiments can be made without departing from the spirit and scope thereof. 

We claim:
 1. A process of making polyalkylene polyamines which comprises condensing an amino compound, said amino compound comprising ammonia, one or more compounds containing nitrogen to which is bonded an active hydrogen or mixtures thereof, in the presence of a metallic phosphate condensation catalyst having a cyclic structure, said condensation catalyst being selected from the group consisting of one or more metallic metaphosphates, metallic ultraphosphates, metallic metaphosphimates, metallic imidophosphates and mixtures thereof.
 2. The process of claim 1 wherein the metal portion of the metallic phosphate condensation catalyst is selected from the group consisting of Group IA, Group IIA, Group IIIB, Group IVB, Group VB, Group VIB, Group VIIB, Group VIII, Group IB, Group IIB, Group IIIA, Group IVA, Group VA, and Group VIA metals and mixtures thereof.
 3. The process of claim 1 wherein the metallic phosphate condensation catalyst comprises a metallic metaphosphate.
 4. The process of claim 3 wherein the metallic metaphosphate comprises sodium trimetaphosphate.
 5. The process of claim 3 wherein the metallic metaphosphate comprises a mixture of sodium trimetaphosphate and sodium tripolyphosphate.
 6. The process of claim 1 wherein the metallic phosphate condensation catalyst is associated with a Group IVB metal oxide or a Group IVA metal oxide.
 7. The process of claim 6 wherein the Group IVB metal oxide comprises a high surface area titanium oxide or zirconium oxide.
 8. The process of claim 6 wherein the Group IVA metal oxide comprises a high surface area silicon oxide.
 9. The process of claim 1 wherein the catalyst has a surface area greater than about 70 m² /gm.
 10. The process of claim 7 wherein the titanium oxide comprises titanium dioxide and the zirconium oxide comprises zirconium dioxide.
 11. The process of claim 8 wherein the silicon oxide comprises silica.
 12. The process of claim 6 wherein the Group IVB metal oxide comprises a mixture of titanium oxide and zirconium oxide.
 13. The process of claim 12 wherein the mixture of titanium oxide and zirconium oxide comprises titanium dioxide and zirconium dioxide.
 14. The process of claim 13 wherein the catalyst has a surface area greater than about 140 m² /gm.
 15. The process of claim 8 wherein the catalyst has a surface area greater than about 70 m² /gm.
 16. The process of claim 1 wherein the catalyst is associated with a support material.
 17. The process of claim 7 wherein the catalyst is associated with a support material.
 18. The process of claim 8 wherein the catalyst is associated with a support material.
 19. The process of claim 16 wherein the support comprises an alumina material or an alumina-silica material.
 20. The process of claim 16 wherein the support comprises a silica material or a silica-alumina material.
 21. The process of claim 17 wherein the support comprises an alumina material or an alumina-silica material.
 22. The process of claim 17 wherein the support comprises a silica material or a silica-alumina material.
 23. The process of claim 18 wherein the support comprises an alumina material or an alumina-silica material,
 24. The process of claim 18 wherein the support comprises a silica material or a silica-alumina material.
 25. The process of claim 16 wherein the support comprises from about 2 to about 60 percent by weight of the catalyst.
 26. The process of claim 17 wherein the support comprises from about 2 to about 60 percent by weight of the catalyst.
 27. The process of claim 18 wherein the support comprises from about 2 to about 60 percent by weight of the catalyst.
 28. The process of claim 1 wherein the catalyst contains a performance moderator.
 29. The process of claim 7 wherein the catalyst contains a performance moderator.
 30. The process of claim 8 wherein the catalyst contains a performance moderator.
 31. The process of claim 28 wherein the performance moderator comprises one or more metal oxides.
 32. The process of claim 29 wherein the performance moderator comprises one or more metal oxides.
 33. The process of claim 30 wherein the performance moderator comprises one or more metal oxides.
 34. The process of claim 31 wherein the performance moderator is selected from the group consisting of one or more Group IA metal oxides, Group IIA metal oxides, Group IIIB metal oxides, Group VB metal oxides, Group VIB metal oxides, Group VIIB metal oxides, Group VIII metal oxides, Group IB metal oxides, Group IIB metal oxides, Group IIIA metal oxides, Group IVA metal oxides, Group VA metal oxides, Group VIA metal oxides, Group IVB metal oxides and mixtures thereof.
 35. The process of claim 34 wherein the performance moderator is selected from the group consisting of one or more oxides of scandium, yttrium, lanthanum, cerium, gadolinium, lutetium, ytterbium, niobium, tantalum, chromium, molybdenum, tungsten, titanium, zirconium, iron, cobalt, nickel, zinc, cadmium, boron, aluminum, gallium, indium, silicon, germanium, tin, lead, arsenic, antimony and bismuth.
 36. The process of claim 32 wherein the performance moderator is selected from the group consisting of one or more Group IA metal oxides, Group IIA metal oxides, Group IIIB metal oxides, Group VB metal oxides, Group VIB metal oxides, Group VIIB metal oxides, Group VIII metal oxides, Group IB metal oxides, Group IIB metal oxides, Group IIIA metal oxides, Group IVA metal oxides, Group VA metal oxides, Group VIA metal oxides, Group IVB metal oxides and mixtures thereof.
 37. The process of claim 36 wherein the performance moderator is selected from the group consisting of one or more oxides of scandium, yttrium, lanthanum, cerium, gadolinium, lutetium, ytterbium, niobium, tantalum, chromium, molybdenum, tungsten, titanium, zirconium, iron, cobalt, nickel, zinc, cadmium, boron, aluminum, gallium, indium, silicon, germanium, tin, lead, arsenic, antimony and bismuth.
 38. The process of claim 33 wherein the performance moderator is selected from the group consisting of one or more Group IA metal oxides, Group IIA metal oxides, Group IIIB metal oxides, Group VB metal oxides, Group VIB metal oxides, Group VIIB metal oxides, Group VIII metal oxides, Group IB metal oxides, Group IIB metal oxides, Group IIIA metal oxides, Group IVA metal oxides, Group VA metal oxides, Group VIA metal oxides, Group IVB metal oxides and mixtures thereof.
 39. The process of claim 38 wherein the performance moderator is selected from the group consisting of one or more oxides of scandium, yttrium, lanthanum, cerium, gadolinium, lutetium, ytterbium, niobium, tantalum, chromium, molybdenum, tungsten, titanium, zirconium, iron, cobalt, nickel, zinc, cadmium, boron, aluminum, gallium, indium, silicon, germanium, tin, lead, arsenic, antimony and bismuth.
 40. The process of claim 28 wherein the performance moderator is selected from the group consisting of a metallic orthophosphate, a metallic pyrophosphate, a metallic polyphosphate, a metallic phosphoramidate, a metallic amidophosphate, and mixtures thereof.
 41. The process of claim 29 wherein the performance moderator is selected from the group consisting of a metallic orthophosphate, a metallic pyrophosphate, a metallic polyphosphate, a metallic phosphoramidate, a metallic amidophosphate, and mixtures thereof.
 42. The process of claim 30 wherein the performance moderator is selected from the group consisting of a metallic orthophosphate, a metallic pyrophosphate, a metallic polyphosphate, a metallic phosphoramidate, a metallic amidophosphate, and mixtures thereof.
 43. The process of claim 28 wherein the performance moderator comprises a mineral acid or a compound derived from a mineral acid.
 44. The process of claim 29 wherein the performance moderator comprises a mineral acid or a compound derived from a mineral acid.
 45. The process of claim 30 wherein the performance moderator comprises a mineral acid or a compound derived from a mineral acid.
 46. The process of claim 43 wherein the performance moderator comprises phosphoric acid or a salt of phosphoric acid.
 47. The process of claim 44 wherein the performance moderator comprises phosphoric acid or a salt of phosphoric acid.
 48. The process of claim 45 wherein the performance moderator comprises phosphoric acid or a salt of phosphoric acid.
 49. The process of claim 43 wherein the performance moderator comprises hydrogen fluoride, hydrofluoric acid or a fluoride salt.
 50. The process of claim 44 wherein the performance moderator comprises hydrogen fluoride, hydrofluoric acid or a fluoride salt.
 51. The process of claim 45 wherein the performance moderator comprises hydrogen fluoride, hydrofluoric acid or a fluoride salt.
 52. The process of claim 43 wherein the performance moderator comprises sulfuric acid or a salt of sulfuric acid.
 53. The process of claim 44 wherein the performance moderator comprises sulfuric acid or a salt or sulfuric acid.
 54. The process of claim 45 wherein the performance moderator comprises sulfuric acid or a salt or sulfuric acid.
 55. The process of claim 6 wherein the Group IVB metal oxide comprises a mixed oxide of a Group IVB metal oxide and one or more other metal oxides.
 56. The process of claim 55 wherein the metal oxide is selected from the group consisting of one or more Group IA metal oxides, Group IIA metal oxides, Group IIIB metal oxides, Group VB metal oxides, Group VIB metal oxides, Group VIIB metal oxides, Group VIII metal oxides, Group IB metal oxides, Group IIB metal oxides, Group IIIA metal oxides, Group IVA metal oxides, Group VA metal oxides, Group VIA metal oxides, other Group IVB metal oxides and mixtures thereof.
 57. The process of claim 55 wherein the metal oxide is selected from the group consisting of one or more oxides of scandium, yttrium, lanthanum, cerium, gadolinium, lutetium, ytterbium, niobium, tantalum, chromium, molybdenum, tungsten, titanium, zirconium, iron, cobalt, nickel, zinc, cadmium, boron, aluminum, gallium, indium, silicon, germanium, tin, lead, arsenic, antimony and bismuth.
 58. The process of claim 1 wherein the Group IVB metal oxide comprises from about 25 weight percent to about 90 weight percent of the weight of the catalyst.
 59. The process of claim 6 wherein the Group IVB metal oxide comprises from about 50 weight percent to about 90 weight percent of the weight of the catalyst,
 60. The process of claim 6 wherein the Group IVB metal oxide comprises from about 75 weight percent to about 90 weight percent of the weight of the catalyst.
 61. The process of claim 1 wherein the amino compound comprises an alkyleneamine.
 62. The process of claim 1 further comprising the addition of an alcohol.
 63. The process of claim 62 wherein the alcohol comprises an alkanolamine or an alkylene glycol.
 64. The process of claim 63 wherein the alkanolamine comprises aminoethylethanolamine.
 65. The process of claim 1 wherein the amino compound comprises a mixture of monoethanolamine and ethylenediamine.
 66. The process of claim 1 wherein the amino compound comprises a mixture of monoethanolamine and diethylenetriamine.
 67. The process to claim 1 wherein the amino compound comprises a mixture of monoethanolamine, ethylenediamine and ammonia.
 68. The process of claim 1 wherein the amino compound comprises a mixture of monoethanolamine, diethylenetriamine and ammonia.
 69. The process of claim 1 wherein the amino compound comprises a mixture of aminoethylethanolamine and ethylenediamine.
 70. The process of claim 1 wherein the amino compound comprises a mixture of aminoethylethanolamine and diethylenetriamine.
 71. The process of claim 1 wherein the amino compound comprises a mixture of aminoethylethanolamine, ethylenediamine and ammonia.
 72. The process of claim 1 wherein the amino compound comprises a mixture of aminoethyl ethanolamine, diethylenetriamine and ammonia.
 73. The process of claim 1 wherein the polyalkylene polyamines product has a TETA+TAEA to PIP+AEP+PEEDA+DAEP+DPE weight ratio of greater than about 0.5, a TETA to TAEA weight ratio of greater than about 2.0 and a TEPA to AETAEA weight ratio of greater than about 2.0.
 74. The polyalkylene polyamines product prepared by the process of claim
 1. 75. The process of claim 1 in which the amines product comprises, based on 100 percent of the weight of the product and exclusive of any water and/or ammonia present,a) greater than about 3.0 weight percent of the combination of TETA and TEPA, b) greater than about 0.1 weight percent of TEPA, c) greater than about 3.0 weight percent of TETA, d) less than about 90.0 weight percent of DETA and/or EDA, e) less than about 90.0 weight percent of MEA and/or AEEA, f) less than about 12.5 weight percent of the combination of PIP and AEP, g) less than about 15.0 weight percent of other polyalkylene polyamines, h) a TETA+TAEA to PIP+AEP+PEEDA+DAEP+DPE weight ratio of greater than about 0.5, i) a TEPA+AETAEA to PIP+AEP+PEEDA+DAEP+DPE+AEPEEDA+iAEPEEDA+AEDAEP+AEDPE+BPEA weight ratio of greater than about 0.5, j) a TETA to TAEA weight ratio of greater than about 2.0, and k) a TEPA to AETAEA weight ratio of greater than about 2.0.
 76. The process of claim 1 wherein the amino compound comprises ethylenediamine in association with ethylene glycol or diethylenetriamine in association with ethylene glycol.
 77. The process of claim 1 wherein the amino compound comprises a mixture of diethanolamine and ethylenediamine or a mixture of diethanolamine and diethylenetriamine.
 78. The process of claim 1 wherein the amino compound comprises a mixture of dihydroxyethylethylenediamine and ethylenediamine or a mixture of dihydroxyethylethylendiamine and diethylenetriamine.
 79. The process of claim 1 wherein the amino compound comprises a mixture of dihydroxyethyldiethylenetriamine and ethylenediamine or a mixture of dihydroxyethyldiethylenetriamine and diethylenetriamine.
 80. The process of claim 1 wherein the amino compound comprises a mixture of dihydroxyethyltriethylenetramine and ethylenediamine or a mixture of dihydroxyethyltriethylenetramine and diethylenetriamine.
 81. The process of claim 3 wherein the metallic metaphosphate comprises sodium tetrametaphosphate.
 82. The process of claim 1 which is effected in the liquid phase, vapor phase, supercritical liquid phase or mixtures thereof.
 83. A process of making alkylamines which comprises contacting an alcohol and at least one of a primary amine, a secondary amine or a tertiary amine in the presence of a metallic phosphate condensation catalyst having a cyclic structure. 